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Excessive Ozonation Stress Triggers Severe Membrane Biofilm Accumulation and Fouling
过度的臭氧应激会引发严重的膜生物膜堆积和结垢IF 11.4SCIEJCI 1.44Q1环境科学与生态学1区Top
- Li Zhang 张丽Li ZhangState Key Laboratory of Environmental Aquatic Chemistry, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing 100085, ChinaMore by Li Zhang
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- Nigel Graham 奈杰尔·格雷厄姆Nigel GrahamDepartment of Civil and Environmental Engineering, Imperial College London, South Kensington Campus, London SW7 2AZ, U.K.More by Nigel Graham
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- Guibai Li 李贵柏Guibai LiState Key Laboratory of Urban Water Resource and Environment (SKLUWRE), School of Environment, Harbin Institute of Technology, Harbin 150090, ChinaMore by Guibai Li
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- Yongguan Zhu 朱永官Yongguan ZhuState Key Laboratory of Urban and Regional Ecology, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing 100085, ChinaMore by Yongguan Zhu
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- Wenzheng Yu* 俞文正*Wenzheng Yu*Email: wzyu@rcees.ac.cnState Key Laboratory of Environmental Aquatic Chemistry, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing 100085, ChinaMore by Wenzheng Yu
Cite this: Environ. Sci. Technol. 2024, XXXX, XXX, XXX-XXX
引用： Environ.Sci. Technol.2024, XXXX, XXX, XXX-XXX
引用： Environ.Sci. Technol.2024, XXXX, XXX, XXX-XXX
© 2024 American Chemical Society
© 2024 美国化学学会
© 2024 美国化学学会
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Abstract 抽象
The established benefits of ozone on microbial pathogen inactivation, natural organic matter degradation, and inorganic/organic contaminant oxidation have favored its application in drinking water treatment. However, viable bacteria are still present after the ozonation of raw water, bringing a potential risk to membrane filtration systems in terms of biofilm accumulation and fouling. In this study, we shed light on the role of the specific ozone dose (0.5 mg-O3/mg-C) in biofilm accumulation during long-term membrane ultrafiltration. Results demonstrated that ozonation transformed the molecular structure of influent dissolved organic matter (DOM), producing fractions that were highly bioavailable at a specific ozone dose of 0.5, which was inferred to be a turning point. With the increase of the specific ozone dose, the biofilm microbial consortium was substantially shifted, demonstrating a decrease in richness and diversity. Unexpectedly, the opportunistic pathogen Legionella was stimulated and occurred in approximately 40% relative abundance at the higher specific ozone dose of 1. Accordingly, the membrane filtration system with a specific ozone dose of 0.5 presented a lower biofilm thickness, a weaker fluorescence intensity, smaller concentrations of polysaccharides and proteins, and a lower Raman activity, leading to a lower hydraulic resistance, compared to that with a specific ozone dose of 1. Our findings highlight the interaction mechanism between molecular-level DOM composition, biofilm microbial consortium, and membrane filtration performance, which provides an in-depth understanding of the impact of ozonation on biofilm accumulation.
臭氧对微生物病原体灭活、天然有机物降解和无机/有机污染物氧化的既定益处有利于其在饮用水处理中的应用。然而，原水臭氧化后仍然存在活菌，给膜过滤系统带来了生物膜积聚和结垢的潜在风险。在这项研究中，我们阐明了特定臭氧剂量（0.5 mg-O 3 / mg-C）在长期膜超滤过程中生物膜积累中的作用。结果表明，臭氧化改变了进水溶解有机物（DOM）的分子结构，在特定臭氧剂量为0.5时产生了具有高度生物利用度的馏分，这被认为是一个转折点。随着特定臭氧剂量的增加，生物膜微生物群落发生了显著变化，显示出丰富度和多样性的下降。出乎意料的是，机会性病原体军团菌受到刺激，在较高的特定臭氧剂量 1 下，相对丰度约为 40%。因此，与特定臭氧剂量为1的膜过滤系统相比，特定臭氧剂量为0.5的膜过滤系统具有较低的生物膜厚度，较弱的荧光强度，较低的多糖和蛋白质浓度以及较低的拉曼活性，导致较低的水力阻力。我们的研究结果突出了分子水平DOM组成、生物膜微生物联合体和膜过滤性能之间的相互作用机制，从而深入了解了臭氧对生物膜积累的影响。
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Synopsis 概要
Excessive ozonation stress triggers severe membrane biofilm accumulation
过度的臭氧化应激会引发严重的膜生物膜积累
1. Introduction 1. 引言
Membrane fouling continues to be a major concern in the application of membrane filtration technology in which the biofilm layer plays a critical role. Various oxidants or disinfectants are commonly used for pretreatment upstream of conventional processes, including membrane separation, and these have been intensively investigated in recent years. (1−4) In terms of the relative benefits of alternative pretreatment methods, involving the inactivation of microbial pathogens, decomposition of natural dissolved organic matter (DOM), oxidation of inorganic contaminants, and the removal of taste-, odor-, and color-causing compounds, ozone is commonly preferred in water treatment. (5) Although microbial levels are difficult to detect due to the rapid reactivity of ozone, viable microbes have been reported to remain present after the ozonation of raw water, (6) offering an opportunity for the formation of biofilm on the surface of subsequent membranes. Several studies have investigated the effect of ozonation on membrane fouling, (7−10) but for the long-term operation of a membrane filtration system, the role of ozone in the biofilm accumulation remains unclear.
膜污染仍然是膜过滤技术应用中的主要问题，其中生物膜层起着关键作用。各种氧化剂或消毒剂通常用于常规工艺的上游预处理，包括膜分离，近年来这些都得到了深入的研究。（1−4） 就替代预处理方法的相对效益而言，包括灭活微生物病原体、分解天然溶解有机物（DOM）、氧化无机污染物以及去除引起味道、气味和颜色的化合物，臭氧在水处理中通常是首选。（5）尽管由于臭氧的快速反应性而难以检测微生物水平，但据报道，在原水臭氧化后，活微生物仍然存在，（6）为在随后的膜表面形成生物膜提供了机会。一些研究已经调查了臭氧化对膜污染的影响（7−10），但对于膜过滤系统的长期运行，臭氧在生物膜积累中的作用尚不清楚。
膜污染仍然是膜过滤技术应用中的主要问题，其中生物膜层起着关键作用。各种氧化剂或消毒剂通常用于常规工艺的上游预处理，包括膜分离，近年来这些都得到了深入的研究。（1−4） 就替代预处理方法的相对效益而言，包括灭活微生物病原体、分解天然溶解有机物（DOM）、氧化无机污染物以及去除引起味道、气味和颜色的化合物，臭氧在水处理中通常是首选。（5）尽管由于臭氧的快速反应性而难以检测微生物水平，但据报道，在原水臭氧化后，活微生物仍然存在，（6）为在随后的膜表面形成生物膜提供了机会。一些研究已经调查了臭氧化对膜污染的影响（7−10），但对于膜过滤系统的长期运行，臭氧在生物膜积累中的作用尚不清楚。
In the process of ozonation, DOM, a highly complex mixture composed of multiple natural and anthropogenic organic molecules, is the major ozone consumer. (11,12) Ozone is able to react with electrophilic functional groups and activated aromatic substances, breaking double bonds, thereby splitting molecules and adding oxygen atoms to molecules. (13,14) Thus, ozone has been shown to lower the aromaticity of DOM by reacting with phenolic moieties found commonly in DOM. (15) Remucal et al. studied molecular-level transformation of two DOM isolates using Orbitrap mass spectrometry and found that, as well as reducing aromaticity, ozonation also decreased the apparent molecular weight and electron donating capacity of DOM with large changes. (16) In addition, ozonation was demonstrated to make organic compounds more hydrophilic and susceptible to biodegradation. (17,18) However, some research studies have shown that ozone may produce reaction byproducts that are less biodegradable and potentially detrimental. (19−21) Therefore, the biodegradability of ozonized DOM, and its potential influence on the subsequent formation and accumulation of biofilm on membrane surfaces, requires further evaluation.
在臭氧化过程中，DOM是一种由多种天然和人为有机分子组成的高度复杂的混合物，是臭氧的主要消耗者。（11,12） 臭氧能够与亲电官能团和活化的芳香族物质发生反应，破坏双键，从而分裂分子并向分子中添加氧原子。（13,14） 因此，臭氧已被证明通过与 DOM 中常见的酚类部分反应来降低 DOM 的芳香性。 （15） Remucal 等人使用 Orbitrap 质谱法研究了两种 DOM 分离物的分子水平转化，发现除了降低芳香性外，臭氧还降低了 DOM 的表观分子量和电子供体能力，并发生了很大的变化。（16） 此外，臭氧化作用被证明使有机化合物更亲水且易生物降解。（17,18） 然而，一些研究表明，臭氧可能产生反应副产物，这些副产物的生物降解性较差，并且可能有害。（19−21） 因此，臭氧DOM的生物降解性及其对膜表面生物膜随后形成和积累的潜在影响需要进一步评估。
在臭氧化过程中，DOM是一种由多种天然和人为有机分子组成的高度复杂的混合物，是臭氧的主要消耗者。（11,12） 臭氧能够与亲电官能团和活化的芳香族物质发生反应，破坏双键，从而分裂分子并向分子中添加氧原子。（13,14） 因此，臭氧已被证明通过与 DOM 中常见的酚类部分反应来降低 DOM 的芳香性。 （15） Remucal 等人使用 Orbitrap 质谱法研究了两种 DOM 分离物的分子水平转化，发现除了降低芳香性外，臭氧还降低了 DOM 的表观分子量和电子供体能力，并发生了很大的变化。（16） 此外，臭氧化作用被证明使有机化合物更亲水且易生物降解。（17,18） 然而，一些研究表明，臭氧可能产生反应副产物，这些副产物的生物降解性较差，并且可能有害。（19−21） 因此，臭氧DOM的生物降解性及其对膜表面生物膜随后形成和积累的潜在影响需要进一步评估。
As a disinfectant, ozone is highly effective in inactivating bacteria in water, (22) but ozone-resistant bacteria can remain after ozonation, which can enhance the accumulation of biofilm on the surface of membranes subsequently. The actively growing microbial species were reported to secrete secondary metabolites that could alter ambient conditions, thus influencing the growth of other microorganisms and shifting relative abundance levels. (23) The variation in the bacterial community is suspected to further affect the biofilm structure and properties, owing to the discrepant extracellular polymeric substances (EPS) secreted. (1,24−26) At present, detailed information regarding the shift of biofilm bacterial community by ozone remains deficient and, moreover, the influence of specific ozone dose, defined as the ratio of ozone dose to dissolved organic carbon in raw water (mg-O3/mg-C), on the microbial composition is also largely unknown.
作为一种消毒剂，臭氧在灭活水中的细菌方面非常有效，（22）但臭氧作用后仍会残留耐臭氧细菌，从而增强膜表面生物膜的积累。据报道，活跃生长的微生物物种会分泌可以改变环境条件的次级代谢物，从而影响其他微生物的生长并改变相对丰度水平。（23）由于分泌的细胞外聚合物（EPS）不同，怀疑细菌群落的变化会进一步影响生物膜的结构和性质。（1,24−26） 目前，关于臭氧对生物膜细菌群落的转移的详细信息仍然不足，此外，特定臭氧剂量（定义为臭氧剂量与原水中溶解有机碳的比率（mg-O 3 /mg-C））对微生物组成的影响也在很大程度上是未知的。
作为一种消毒剂，臭氧在灭活水中的细菌方面非常有效，（22）但臭氧作用后仍会残留耐臭氧细菌，从而增强膜表面生物膜的积累。据报道，活跃生长的微生物物种会分泌可以改变环境条件的次级代谢物，从而影响其他微生物的生长并改变相对丰度水平。（23）由于分泌的细胞外聚合物（EPS）不同，怀疑细菌群落的变化会进一步影响生物膜的结构和性质。（1,24−26） 目前，关于臭氧对生物膜细菌群落的转移的详细信息仍然不足，此外，特定臭氧剂量（定义为臭氧剂量与原水中溶解有机碳的比率（mg-O 3 /mg-C））对微生物组成的影响也在很大程度上是未知的。
The DOM provides substrates serving as niches for the biofilm microbes and they are major energy sources supporting microbial growth. (27) The variation in the molecular composition of DOM has been reported to affect the diversity, structure, and functioning of microbial communities. (28,29) In turn, microbial consortia produce chemo-diversity by degrading larger molecules into smaller structures and releasing new molecules into the water. (30) The interactions between chemo-diversity and biodiversity are complex but vitally important. Several previous studies have investigated natural ecosystems and endeavored to disclose the interaction mechanisms. In a pelagic marine system, Osterholz et al. found that the active microbial community correlated with specific DOM molecular formulas and the trend was most pronounced at the species level. (31) Tanentzap and co-workers focused on a fresh water system and they discovered that the chemical and microbial diversities were positively correlated, with DOM having a stronger effect on microbes than vice versa. (27) However, less attention has been paid to the engineering system, and the interactions between DOM and biofilm microbial consortia remain unknown, which are of particular importance since they likely have a pronounced effect on biofilm accumulation and membrane filtration performance.
DOM为生物膜微生物提供了作为生态位的基质，它们是支持微生物生长的主要能源。（27）据报道，DOM分子组成的变化会影响微生物群落的多样性、结构和功能。（28,29） 反过来，微生物联盟通过将较大的分子降解为较小的结构并将新分子释放到水中来产生化学多样性。（30）化学多样性与生物多样性之间的相互作用是复杂的，但至关重要。之前的几项研究已经调查了自然生态系统，并试图揭示其相互作用机制。在远洋海洋系统中，Osterholz等人发现，活跃的微生物群落与特定的DOM分子式相关，并且这种趋势在物种水平上最为明显。（31）Tanentzap及其同事专注于淡水系统，他们发现化学和微生物多样性呈正相关，DOM对微生物的影响比反之亦然。（27）然而，对工程系统的关注较少，DOM与生物膜微生物联盟之间的相互作用仍然未知，因为它们可能对生物膜积累和膜过滤性能有显著影响，因此特别重要。
DOM为生物膜微生物提供了作为生态位的基质，它们是支持微生物生长的主要能源。（27）据报道，DOM分子组成的变化会影响微生物群落的多样性、结构和功能。（28,29） 反过来，微生物联盟通过将较大的分子降解为较小的结构并将新分子释放到水中来产生化学多样性。（30）化学多样性与生物多样性之间的相互作用是复杂的，但至关重要。之前的几项研究已经调查了自然生态系统，并试图揭示其相互作用机制。在远洋海洋系统中，Osterholz等人发现，活跃的微生物群落与特定的DOM分子式相关，并且这种趋势在物种水平上最为明显。（31）Tanentzap及其同事专注于淡水系统，他们发现化学和微生物多样性呈正相关，DOM对微生物的影响比反之亦然。（27）然而，对工程系统的关注较少，DOM与生物膜微生物联盟之间的相互作用仍然未知，因为它们可能对生物膜积累和膜过滤性能有显著影响，因此特别重要。
In this paper, we present new information that sheds light on the molecular-level DOM composition at varying specific ozone doses, the biofilm microbial structure, interactions between DOM chemo-diversity and biofilm biodiversity and, importantly, decipher the associated influencing mechanism on membrane filtration performance. Here, Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR-MS), the state-of-the-art analytical tool for molecular-level DOM characterization, was employed in the experiments, owing to its high resolution, sensitivity, and mass accuracy. (31) We hypothesize that the composition of DOM is substantially transformed, depending on the value of the specific ozone dose. With the increase of the specific ozone dose, the biofilm biodiversity presents a declining trend. The synergistic effect of DOM and biofilm microbial consortia may contribute to the differences in the membrane filtration performance. The objective of the study, described subsequently, was to provide in-depth insight into the role of specific ozone dose in biofilm formation and the interactions between DOM, biofilm bacterial community, and membrane filtration performance.
在本文中，我们提出了新的信息，揭示了不同特定臭氧剂量下的分子水平DOM组成，生物膜微生物结构，DOM化学多样性与生物膜生物多样性之间的相互作用，重要的是，破译了膜过滤性能的相关影响机制。在这里，傅里叶变换离子回旋共振质谱（FT-ICR-MS）因其高分辨率、高灵敏度和质量精度而被用于实验，这是用于分子水平DOM表征的最先进的分析工具。（31）我们假设DOM的组成发生了实质性的变化，这取决于特定臭氧剂量的值。随着特定臭氧剂量的增加，生物膜生物多样性呈现下降趋势。DOM和生物膜微生物联盟的协同作用可能导致膜过滤性能的差异。随后描述的这项研究的目的是深入了解特定臭氧剂量在生物膜形成中的作用以及 DOM、生物膜细菌群落和膜过滤性能之间的相互作用。
在本文中，我们提出了新的信息，揭示了不同特定臭氧剂量下的分子水平DOM组成，生物膜微生物结构，DOM化学多样性与生物膜生物多样性之间的相互作用，重要的是，破译了膜过滤性能的相关影响机制。在这里，傅里叶变换离子回旋共振质谱（FT-ICR-MS）因其高分辨率、高灵敏度和质量精度而被用于实验，这是用于分子水平DOM表征的最先进的分析工具。（31）我们假设DOM的组成发生了实质性的变化，这取决于特定臭氧剂量的值。随着特定臭氧剂量的增加，生物膜生物多样性呈现下降趋势。DOM和生物膜微生物联盟的协同作用可能导致膜过滤性能的差异。随后描述的这项研究的目的是深入了解特定臭氧剂量在生物膜形成中的作用以及 DOM、生物膜细菌群落和膜过滤性能之间的相互作用。
2. Materials and Methods 2. 材料与方法
2.1. Experiment setup and Operation
2.1. 实验设置和操作
Water samples were collected from River Jingmi (Beijing, China), which serves as the source of the drinking water supply for the large majority of the citizens living in Beijing. Polyvinylidene fluoride ultrafiltration membrane (Beijing Separate Equipment Co., Ltd., China), with a nominal molecular cutoff of 100 kDa, and an area of approximately 78.5 cm2, was selected for the experiments. A gravity-driven membrane filtration system, with a constant transmembrane pressure of 35 mbar (35 cm water head), was adopted as the experimental model due to its advantages in terms of biofilm robustness. Further detailed information concerning the surface water characteristics and filtration system is given in the Supporting Information (SI, Table S1 and Figure S1).
水样采集自京密河（中国北京），京密河是北京绝大多数市民的饮用水供应来源。选取标称分子截止值为100 kDa，面积约78.5 cm 2 的聚偏氟乙烯超滤膜（中国北京分离设备有限公司）。采用重力驱动的膜过滤系统，其恒定跨膜压力为35 mbar（35 cm水头），因其在生物膜鲁棒性方面的优势而作为实验模型。有关地表水特性和过滤系统的更多详细信息，请参阅支持信息（SI，表S1和图S1）。
水样采集自京密河（中国北京），京密河是北京绝大多数市民的饮用水供应来源。选取标称分子截止值为100 kDa，面积约78.5 cm 2 的聚偏氟乙烯超滤膜（中国北京分离设备有限公司）。采用重力驱动的膜过滤系统，其恒定跨膜压力为35 mbar（35 cm水头），因其在生物膜鲁棒性方面的优势而作为实验模型。有关地表水特性和过滤系统的更多详细信息，请参阅支持信息（SI，表S1和图S1）。
Surface water was ozonized with fresh gaseous ozone generated from pure oxygen by a laboratory ozone generator (ZA-10G-C, HangMu, China). The gas contacting apparatus was operated under 0.1 kPa pressure and the ozone was added under vigorous mixing on the basis of bubble size, to yield specific doses of 0.5 mg-O3/mg-C and 1 mg-O3/mg-C, which were ratios representative of practical applications and verified using the standard indigo method. (32) The ozonized samples were stored at room temperature for 20 h to allow for complete ozone consumption and decay. Thereafter, water samples serving as feed waters were added to the filtration systems. For convenience, the filtration systems with specific ozone doses of 0.5 mg-O3/mg-C and 1 mg-O3/mg-C were denoted as ratio 0.5 and ratio 1, respectively.
地表水由实验室臭氧发生器（ZA-10G-C，中国杭木）用纯氧产生的新鲜气态臭氧进行臭氧处理。气体接触装置在0.1 kPa压力下运行，根据气泡大小在剧烈混合下加入臭氧，得到比剂量0.5 mg-O 3 /mg-C和1 mg-O 3 /mg-C，这是代表实际应用的比例，并使用标准靛蓝方法进行验证。（32）将臭氧样品在室温下储存20小时，以允许臭氧完全消耗和衰变。此后，作为给水的水样被添加到过滤系统中。为方便起见，臭氧比剂量为0.5 mg-O 3 /mg-C和1 mg-O 3 /mg-C的过滤系统分别表示为比率0.5和比率1。
地表水由实验室臭氧发生器（ZA-10G-C，中国杭木）用纯氧产生的新鲜气态臭氧进行臭氧处理。气体接触装置在0.1 kPa压力下运行，根据气泡大小在剧烈混合下加入臭氧，得到比剂量0.5 mg-O 3 /mg-C和1 mg-O 3 /mg-C，这是代表实际应用的比例，并使用标准靛蓝方法进行验证。（32）将臭氧样品在室温下储存20小时，以允许臭氧完全消耗和衰变。此后，作为给水的水样被添加到过滤系统中。为方便起见，臭氧比剂量为0.5 mg-O 3 /mg-C和1 mg-O 3 /mg-C的过滤系统分别表示为比率0.5和比率1。
2.2. DOM Preparation for ESI-FT-ICR-MS Measurement and Data Analyses
2.2. ESI-FT-ICR-MS测量和数据分析的DOM准备
To desalinate and concentrate DOM, solid phase extraction was performed on all of the influent samples using Bond Elute PPL cartridges (200 mg, 3 mL; Agilent Technologies, USA) according to the method of Dittmar et al. (33) Briefly, the cartridges were rinsed with 3 mL of methanol (MS grade) prior to use. An acidified sample was passed through the cartridge, rinsed with three cartridge volumes of 0.01 M HCl, dried with ultrapure N2, and immediately extracted with two cartridge volumes of methanol (MS grade). The eluates were blow-dried with ultrapure N2 and redissolved in a 1 mL mixture of 1:1 (v/v) methanol/ultrapure water. The samples were re-filtered with 0.2 μm PTFE syringe filters pre-rinsed with a 1:1 mixture of methanol to ultrapure water. All samples were adjusted to an equal mass concentration of 100 mg-C·L–1, to eliminate the influence of concentration on the ionization efficiency of molecules detected. (34,35) The extraction efficiency exceeded 75% using this method. (36) Each sample was examined in duplicate according to the methods reported previously. (37,38) A blank sample for the sorbent was obtained by extracting ultrapure water with the same procedures and volumes as those for the samples.
为了淡化和浓缩 DOM，使用 Bond Elute PPL 小柱（200 mg，3 mL;Agilent Technologies，USA）根据Dittmar等人的方法（33）简言之，在使用前用3 mL甲醇（MS级）冲洗滤芯。将酸化的样品通过滤芯，用三个滤芯体积的0.01 M HCl冲洗，用超纯氮 2 干燥，并立即用两个滤芯体积的甲醇（MS级）萃取。洗脱液用超纯氮 2 吹干，并重新溶解在1 mL 1：1 （v/v）甲醇/超纯水的混合物中。用0.2μmPTFE注射器过滤器重新过滤样品，并用甲醇与超纯水的1：1混合物预冲洗。将所有样品调节至等量浓度100 mg-C·L –1 ，以消除浓度对被检测分子电离效率的影响。（34,35） 使用该方法提取效率超过75%。（36） 根据先前报告的方法，对每个样品进行一式两份的检查。（37,38）通过提取超纯水，以与样品相同的程序和体积获得吸附剂的空白样品。
为了淡化和浓缩 DOM，使用 Bond Elute PPL 小柱（200 mg，3 mL;Agilent Technologies，USA）根据Dittmar等人的方法（33）简言之，在使用前用3 mL甲醇（MS级）冲洗滤芯。将酸化的样品通过滤芯，用三个滤芯体积的0.01 M HCl冲洗，用超纯氮 2 干燥，并立即用两个滤芯体积的甲醇（MS级）萃取。洗脱液用超纯氮 2 吹干，并重新溶解在1 mL 1：1 （v/v）甲醇/超纯水的混合物中。用0.2μmPTFE注射器过滤器重新过滤样品，并用甲醇与超纯水的1：1混合物预冲洗。将所有样品调节至等量浓度100 mg-C·L –1 ，以消除浓度对被检测分子电离效率的影响。（34,35） 使用该方法提取效率超过75%。（36） 根据先前报告的方法，对每个样品进行一式两份的检查。（37,38）通过提取超纯水，以与样品相同的程序和体积获得吸附剂的空白样品。
Ultrahigh resolution mass spectra were obtained using a solariX FT-ICR-MS instrument (Bruker Daltonik GmbH, Germany) equipped with a 15.0 T superconducting magnet and an ESI ion source under negative ion mode. The details for mass spectra acquirement, calibration, and peak assignment can be found in Supporting Information. Ratios O/C ≤ 1.2 and 0.2 ≤ H/C ≤ 2.3 were used as the further restrictions for the formula calculation. (39) Seven compound groups were delineated by the H/C and O/C cutoffs in the van Krevelen diagrams, according to a previous publication. (40) To further characterize the molecular properties of DOM, aromaticity index (AI), which indicates the fraction of aromatic and condensed aromatic structures, (41) and nominal oxidation state of carbon (NOSC), which is related to the bioavailability of the molecule, (42) were calculated by the following equations
使用配备 15.0 T 超导磁体和 ESI 离子源的 solariX FT-ICR-MS 仪器（Bruker Daltonik GmbH，德国）在负离子模式下获得超高分辨率质谱。有关质谱采集、校准和峰分配的详细信息，请参阅支持信息。比率 O/C ≤ 1.2 和 0.2 ≤ H/C ≤ 2.3 被用作公式计算的进一步限制。（39） 根据先前的出版物，van Krevelen 图中的 H/C 和 O/C 截止值描绘了七个化合物基团。（40）为了进一步表征DOM的分子性质，通过以下公式计算了表示芳香族和缩合芳香族结构比例的芳香指数（AI）（41）和与分子生物利用度相关的碳的标称氧化态（NOSC）（42）where c, h, o, n, and s refer to the stoichiometric number of carbon, hydrogen, oxygen, nitrogen, and sulfur atoms per formula, respectively. Significant differences were determined using the Kruskal–Wallis test.
其中 C、H、O、N 和 S 分别表示每个公式中碳、氢、氧、氮和硫原子的化学计量数。使用 Kruskal-Wallis 检验确定显着差异。
使用配备 15.0 T 超导磁体和 ESI 离子源的 solariX FT-ICR-MS 仪器（Bruker Daltonik GmbH，德国）在负离子模式下获得超高分辨率质谱。有关质谱采集、校准和峰分配的详细信息，请参阅支持信息。比率 O/C ≤ 1.2 和 0.2 ≤ H/C ≤ 2.3 被用作公式计算的进一步限制。（39） 根据先前的出版物，van Krevelen 图中的 H/C 和 O/C 截止值描绘了七个化合物基团。（40）为了进一步表征DOM的分子性质，通过以下公式计算了表示芳香族和缩合芳香族结构比例的芳香指数（AI）（41）和与分子生物利用度相关的碳的标称氧化态（NOSC）（42）
(1)
(2)
其中 C、H、O、N 和 S 分别表示每个公式中碳、氢、氧、氮和硫原子的化学计量数。使用 Kruskal-Wallis 检验确定显着差异。
2.3. DOM Physicochemical Properties
2.3. DOM理化性质
2.3.1. Fluorescence Characteristic
2.3.1. 荧光特性
An excitation–emission matrix (EEM) fluorescence spectrometer (F-4600, Hitachi, Japan) was employed for the analysis of the fluorescence properties of samples (water and biofilm). A volume of 15 mL of 0.1 M NaCl solution was used to rinse the biofilm from the membrane surface. The sample EEM spectra were blank subtracted, and the intensities were normalized by the ultrapure water Raman peak at an excitation of 350 nm (386–410 nm emission), converting fluorescence data to Raman units (R.U.). (43) First- and second-order Rayleigh scatters were removed from the EEM spectra. Each sample was measured in triplicate, and the results were averaged.
使用激发发射矩阵（EEM）荧光光谱仪（F-4600，日立，日本）分析样品（水和生物膜）的荧光特性。使用体积为 15 mL 的 0.1 M NaCl 溶液冲洗膜表面的生物膜。将样品EEM光谱减去空白，在350 nm激发（386–410 nm发射）下通过超纯水拉曼峰对强度进行归一化，将荧光数据转换为拉曼单位（R.U.）。（43）从EEM光谱中去除了一阶和二阶瑞利散射。每个样本一式三份，并对结果进行平均。
使用激发发射矩阵（EEM）荧光光谱仪（F-4600，日立，日本）分析样品（水和生物膜）的荧光特性。使用体积为 15 mL 的 0.1 M NaCl 溶液冲洗膜表面的生物膜。将样品EEM光谱减去空白，在350 nm激发（386–410 nm发射）下通过超纯水拉曼峰对强度进行归一化，将荧光数据转换为拉曼单位（R.U.）。（43）从EEM光谱中去除了一阶和二阶瑞利散射。每个样本一式三份，并对结果进行平均。
2.3.2. Apparent Molecular Weight Distribution
2.3.2. 表观分子量分布
The apparent molecular weight of the sample organic matter was determined using a high-performance size exclusion chromatography, with an operating wavelength of 254 nm. Based on the apparent molecular weight profile obtained using sodium polystyrenesulfonate as a standard, the correlation between retention time and apparent molecular weight was determined. Accordingly, the apparent molecular weight distribution profiles of the sample were ascertained. All samples were pre-filtered by a 0.22 μm syringe filter before being injected into the instrument.
使用高效尺寸排阻色谱法测定样品有机物的表观分子量，工作波长为254 nm。基于以聚苯乙烯磺酸钠为标准品获得的表观分子量曲线，确定了保留时间与表观分子量之间的相关性。因此，确定了样品的表观分子量分布曲线。所有样品在进样到仪器之前都经过 0.22 μm 注射器过滤器的预过滤。
使用高效尺寸排阻色谱法测定样品有机物的表观分子量，工作波长为254 nm。基于以聚苯乙烯磺酸钠为标准品获得的表观分子量曲线，确定了保留时间与表观分子量之间的相关性。因此，确定了样品的表观分子量分布曲线。所有样品在进样到仪器之前都经过 0.22 μm 注射器过滤器的预过滤。
2.3.3. Chemical Bonds Linking the Molecules
2.3.3. 连接分子的化学键
X-ray photoelectron spectroscopy (XPS; PHI Quantera II, ULVAC, Japan) measurements were conducted with a Thermo Escalab 250 electron spectrometer using 150 W Al-Kα radiation, yielding the identification of chemical compositions and oxidation states of elements on the freeze-dried biofilm surface. A Fourier transform infrared (FTIR) spectrometer (Spectrum Two, PerkinElmer, USA) with an attenuated total reflectance accessory was used to analyze the functional groups of freeze–dried biofilm. A Raman spectrometer (inVia-Reflex, Renishaw, UK) was employed to reveal the Raman activity of the freeze-dried biofilm, with a wavelength of 532 nm and a 50× ultra-long working distance objective lens. At least five randomized locations were selected for the measurement. The XPS spectra were further fitted by XPSPEAK software, and all the spectral curves were plotted with Origin 2021 software.
X射线光电子能谱（XPS;PHI Quantera II， ULVAC， Japan）使用 Thermo Escalab 250 电子能谱仪使用 150 W Al-Kα 辐射进行测量，从而鉴定了冻干生物膜表面元素的化学成分和氧化态。使用带有衰减全反射附件的傅里叶变换红外 （FTIR） 光谱仪（Spectrum Two，PerkinElmer，USA）分析冻干生物膜的官能团。采用拉曼光谱仪（inVia-Reflex，Renishaw，UK）揭示了冻干生物膜的拉曼活性，波长为532 nm，超长工作距离物镜为50×。至少选择了五个随机位置进行测量。XPS光谱通过XPSPEAK软件进一步拟合，所有光谱曲线均使用Origin 2021软件绘制。
X射线光电子能谱（XPS;PHI Quantera II， ULVAC， Japan）使用 Thermo Escalab 250 电子能谱仪使用 150 W Al-Kα 辐射进行测量，从而鉴定了冻干生物膜表面元素的化学成分和氧化态。使用带有衰减全反射附件的傅里叶变换红外 （FTIR） 光谱仪（Spectrum Two，PerkinElmer，USA）分析冻干生物膜的官能团。采用拉曼光谱仪（inVia-Reflex，Renishaw，UK）揭示了冻干生物膜的拉曼活性，波长为532 nm，超长工作距离物镜为50×。至少选择了五个随机位置进行测量。XPS光谱通过XPSPEAK软件进一步拟合，所有光谱曲线均使用Origin 2021软件绘制。
2.4. Biofilm Morphological Structure
2.4. 生物膜形态结构
At the end of the experiments, the biofilms together with the membranes were gently taken out of the filtration apparatus and were then cut into several pieces. Sections of pieces were directly freeze-dried using a lyophilizer (Scientz-18N, China). Both surface and cross-sectional images were captured using a high-resolution field emission gun scanning electron microscope (SEM; S-4800, Hitachi, Japan). Fresh biofilms were analyzed with InfiniteFocus (G5, Alicona, Austria), which is a flexible optical 3D measurement instrument, yielding information on the optical micrographs and roughness data simultaneously.
在实验结束时，将生物膜和膜一起轻轻地从过滤装置中取出，然后切成几块。使用冻干机（Scientz-18N，中国）直接冻干切片。使用高分辨率场发射枪扫描电子显微镜（SEM;S-4800，日立，日本）。使用InfiniteFocus（G5，Alicona，Austria）分析新鲜生物膜，这是一种灵活的光学3D测量仪器，可同时产生光学显微照片和粗糙度数据的信息。
在实验结束时，将生物膜和膜一起轻轻地从过滤装置中取出，然后切成几块。使用冻干机（Scientz-18N，中国）直接冻干切片。使用高分辨率场发射枪扫描电子显微镜（SEM;S-4800，日立，日本）。使用InfiniteFocus（G5，Alicona，Austria）分析新鲜生物膜，这是一种灵活的光学3D测量仪器，可同时产生光学显微照片和粗糙度数据的信息。
2.5. Biofilm DNA Extraction, Sequencing, and Statistical Analyses
2.5. 生物膜DNA提取、测序和统计分析
The biofilm DNA was extracted from an area of ∼2 cm2, using proteinase K and SDS-based lysis, and purified with DNA Clean & Concentrator-25 Kit (ZYMO RESEARCH, USA) according to the manufacturer’s protocol. Three areas were selected for each sample in the microbial consortium analysis. Universal primers, containing 515 forward (5′-GTGCCAGCMGCCGCGGTAA-3′) and 806 reverse (5′-GGACTACHVGGGTWTCTAAT-3′), were used to amplify the V4 region of bacterial 16S rRNA genes. Three areas of the same size were selected for each biofilm. All amplified genes were sequenced by an Illumina MiSeq sequencer. Further detailed information concerning the amplification methods and data processing procedures is given in Supporting Information. The raw sequencing data were deposited to the sequence read archive database of the National Center of Biotechnology Information (NCBI) under accession number PRJNA970303.
使用基于蛋白酶K和SDS的裂解从∼2厘米 2 的区域提取生物膜DNA，并根据制造商的方案用DNA Clean&Concentrator-25试剂盒（ZYMO RESEARCH，USA）纯化。在微生物联盟分析中，为每个样品选择了三个区域。使用含有 515 个正向 （5′-GTGCCAGCMGCCGCGGTAA-3′） 和 806 个反向 （5′-GGACTACHVGGGTWTCTAAT-3′） 的通用引物扩增细菌 16S rRNA 基因的 V4 区域。为每个生物膜选择三个相同大小的区域。所有扩增的基因均由Illumina MiSeq测序仪测序。有关扩增方法和数据处理程序的更多详细信息，请参阅支持信息。原始测序数据被存入美国国家生物技术信息中心（NCBI）的序列读取存档数据库，登录号为PRJNA970303。
使用基于蛋白酶K和SDS的裂解从∼2厘米 2 的区域提取生物膜DNA，并根据制造商的方案用DNA Clean&Concentrator-25试剂盒（ZYMO RESEARCH，USA）纯化。在微生物联盟分析中，为每个样品选择了三个区域。使用含有 515 个正向 （5′-GTGCCAGCMGCCGCGGTAA-3′） 和 806 个反向 （5′-GGACTACHVGGGTWTCTAAT-3′） 的通用引物扩增细菌 16S rRNA 基因的 V4 区域。为每个生物膜选择三个相同大小的区域。所有扩增的基因均由Illumina MiSeq测序仪测序。有关扩增方法和数据处理程序的更多详细信息，请参阅支持信息。原始测序数据被存入美国国家生物技术信息中心（NCBI）的序列读取存档数据库，登录号为PRJNA970303。
To reveal the commonness and discrepancy in the bacterial communities of different biofilms, an UpSet plot was drawn based on the ASVs data with the R package {UpSetR}. To investigate the changes in the relative abundance of bacterial taxa under different conditions, we deciphered the taxonomic composition at the phylum and genus levels. The chord chart was delineated with R packages {circlize} and {statnet}, and the bar plot was completed by Origin 2021. To evaluate whether differences existed in the bacterial communities under different conditions, principal coordinate analysis (PCoA) was performed (R package {vegan}). To quantify the discrepancies between bacterial communities, a boxplot was drawn based on the Bray–Curtis dissimilarity matrix using Origin 2021. Significant differences were determined using the Kruskal–Wallis test.
为了揭示不同生物膜细菌群落的共性和差异性，基于 R 包 {UpSetR} 的 ASV 数据绘制了 UpSet 图。为了研究不同条件下细菌类群相对丰度的变化，我们破译了门和属水平的分类组成。弦图用 R 包 {circlize} 和 {statnet} 描绘，条形图由 Origin 2021 完成。为了评估不同条件下细菌群落是否存在差异，进行了主坐标分析（PCoA）（R 包 {vegan}）。为了量化细菌群落之间的差异，使用 Origin 2021 根据 Bray-Curtis 差异矩阵绘制了一个箱线图。使用 Kruskal-Wallis 检验确定显着差异。
为了揭示不同生物膜细菌群落的共性和差异性，基于 R 包 {UpSetR} 的 ASV 数据绘制了 UpSet 图。为了研究不同条件下细菌类群相对丰度的变化，我们破译了门和属水平的分类组成。弦图用 R 包 {circlize} 和 {statnet} 描绘，条形图由 Origin 2021 完成。为了评估不同条件下细菌群落是否存在差异，进行了主坐标分析（PCoA）（R 包 {vegan}）。为了量化细菌群落之间的差异，使用 Origin 2021 根据 Bray-Curtis 差异矩阵绘制了一个箱线图。使用 Kruskal-Wallis 检验确定显着差异。
2.6. Hydraulic Resistance of Filtration System
2.6. 过滤系统的液压阻力
The total hydraulic resistance (Rt, [m–1]) was calculated as
总水力阻力（R t ，[m –1 ]）计算公式为：where μ is the dynamic viscosity of water at a given temperature [Pa·s], TMP is the transmembrane pressure [Pa], and J is the permeate flux of the membrane filtration system [L·m–2·h–1] and was calculated using the following equation
其中μ是给定温度下水的动态粘度[Pa·s]，TMP是跨膜压力[Pa]，J是膜过滤系统的渗透通量[L·m –2 ·h –1 ]，使用以下公式计算where ΔV is the change of permeate volume [L], A is the filtration area [m2], and ΔT is the change of time [h].
其中ΔV是渗透体积的变化[L]，A是过滤面积[m 2 ]，ΔT是时间的变化[h]。
总水力阻力（R t ，[m –1 ]）计算公式为：
(3)
其中μ是给定温度下水的动态粘度[Pa·s]，TMP是跨膜压力[Pa]，J是膜过滤系统的渗透通量[L·m –2 ·h –1 ]，使用以下公式计算
(4)
其中ΔV是渗透体积的变化[L]，A是过滤面积[m 2 ]，ΔT是时间的变化[h]。
3. Results and Discussion
3. 结果与讨论
3.1. Molecular-level Transformation of DOM by Ozonation
3.1. DOM的臭氧分子转化
To investigate the molecular-level composition and variation of DOM, a van Krevelen diagram was plotted according to the acquired ESI-FT-ICR spectra (Supporting Information Figure S2). As displayed by the van Krevelen diagram, based on the element ratios of O/C and H/C (Figure 1A), the DOM was categorized into seven molecular classes. According to the differential distribution profiles of molecular formulas, the variation in DOM molecules across different influents can be seen visually (Figure 1B–D). Regionally, as a function of increasing specific ozone dose, the molecules with lipid-, unsaturated hydrocarbon-, and lignin-like structures showed a decreased, but then increased, tendency (Figure 1E). In contrast, for the aliphatic-like, carbohydrate-like, tannin-like, and condensed aromatic molecules, an opposite trend was observed (Figure 1E). The selective transformation of compounds by ozone through electrophilic substitution and hydroxylation was suspected to be the principal contributor to the observed effects. (12,44) In addition, the transformation between the molecules could also account for the generated differences. The conversion from lipid- and lignin-like compounds to condensed aromatic substances provided a convincing explanation for the contrary variation behavior during ozonation. (45)
为了研究DOM的分子水平组成和变化，根据采集的ESI-FT-ICR谱图绘制了van Krevelen图（支持信息图S2）。如van Krevelen图所示，根据O / C和H / C的元素比率（图1A），DOM分为七个分子类别。根据分子式的差异分布曲线，可以直观地看到不同进水剂中DOM分子的变化（图1B-D）。从区域上看，作为增加特定臭氧剂量的函数，具有脂质、不饱和碳氢化合物和木质素样结构的分子显示出下降的趋势，但随后增加（图1E）。相反，对于脂肪族分子、碳水化合物族分子、单宁族分子和缩合芳香族分子，观察到相反的趋势（图1E）。臭氧通过亲电取代和羟基化对化合物的选择性转化被怀疑是观察到效应的主要贡献者。（12,44）此外，分子之间的转化也可以解释产生的差异。从脂质和木质素样化合物向缩合芳香物质的转化为臭氧化过程中的相反变化行为提供了令人信服的解释。(45)
为了研究DOM的分子水平组成和变化，根据采集的ESI-FT-ICR谱图绘制了van Krevelen图（支持信息图S2）。如van Krevelen图所示，根据O / C和H / C的元素比率（图1A），DOM分为七个分子类别。根据分子式的差异分布曲线，可以直观地看到不同进水剂中DOM分子的变化（图1B-D）。从区域上看，作为增加特定臭氧剂量的函数，具有脂质、不饱和碳氢化合物和木质素样结构的分子显示出下降的趋势，但随后增加（图1E）。相反，对于脂肪族分子、碳水化合物族分子、单宁族分子和缩合芳香族分子，观察到相反的趋势（图1E）。臭氧通过亲电取代和羟基化对化合物的选择性转化被怀疑是观察到效应的主要贡献者。（12,44）此外，分子之间的转化也可以解释产生的差异。从脂质和木质素样化合物向缩合芳香物质的转化为臭氧化过程中的相反变化行为提供了令人信服的解释。(45)
Figure 1 图1
Figure 1. Molecular-level DOM compositional patterns of the influents. (A) Regions of the van Krevelen diagram based on ratios of O/C and H/C. (B–D) Van Krevelen diagrams of influent DOM in the control, ratio 0.5, and ratio 1 membrane filtration systems, respectively. (E) Regional proportion of the DOM molecules. (F) Venn diagram of the molecular DOM formulas shared in the different samples. (G) Proportion of CHO, CHON, CHOS, and CHONS molecules in control, ratio 0.5, and ratio 1 influents. (H,I) Distribution of AI and NOSC values for molecular formulas of the influent DOM, respectively. Significant differences were investigated using the Kruskal–Wallis test. The marks a, b, and c in bold indicate statistical significance at P < 0.05.
图 1.进水物的分子水平DOM组成模式。（A） 基于 O/C 和 H/C 比率的 van Krevelen 图的区域。 （b–D） 分别是控制、比率 0.5 和比率 1 膜过滤系统中进水 DOM 的 Van Krevelen 图。（E） DOM分子的区域比例。（F） 不同样品中共享的分子DOM分子式的维恩图。（G） 对照组 CHO、CHON、CHOS 和 CHONS 分子的比例，比例为 0.5，比例为 1。（H，I）进水DOM分子式AI和NOSC值的分布。使用 Kruskal-Wallis 检验研究了显着差异。粗体标记 a、b 和 c 表示 P < 0.05 时的统计学显著性。
As shown by the Venn diagram (Figure 1F), a total of 256 formulas were unaffected by specific ozone dose and presented in all the samples. Interestingly, the number of formulas shared by the control/ratio 1 group (1784) was larger than that by the control/ratio 0.5 (369) and ratio 0.5/ratio 1 groups (488). Moreover, for the classified CHO, CHON, CHOS, and CHONS molecules, CHO species appeared more dominant in both the control and ratio 1 cases than other species; whereas for the ratio 0.5 case, the CHOS compound occupied the largest percentage (Figure 1G). These results imply that the specific ozone dose of 0.5 may be a turning point in the ozonation process.
如维恩图（图1F）所示，共有256个配方不受特定臭氧剂量的影响，并出现在所有样品中。有趣的是，对照/比率 1 组 （1784） 共享的公式数量大于对照/比率 0.5 （369） 和比率 0.5/比率 1 组 （488） 的公式数量。此外，对于分类的CHO、CHON、CHOS、CHONS分子，CHO物种在对照和比例1病例中均比其他物种更显明显;而对于比率为0.5的情况，CHOS化合物占据了最大的百分比（图1G）。这些结果表明，0.5的特定臭氧剂量可能是臭氧化过程的一个转折点。
如维恩图（图1F）所示，共有256个配方不受特定臭氧剂量的影响，并出现在所有样品中。有趣的是，对照/比率 1 组 （1784） 共享的公式数量大于对照/比率 0.5 （369） 和比率 0.5/比率 1 组 （488） 的公式数量。此外，对于分类的CHO、CHON、CHOS、CHONS分子，CHO物种在对照和比例1病例中均比其他物种更显明显;而对于比率为0.5的情况，CHOS化合物占据了最大的百分比（图1G）。这些结果表明，0.5的特定臭氧剂量可能是臭氧化过程的一个转折点。
With regard to the calculated AI value, it also demonstrated a significantly lower median for the ratio 0.5 case (0.179) than for other ozonation treatments (0.313 and 0.281 for control and ratio 1 cases, respectively), which further indicated the transitional role of the specific ozone dose at 0.5 in the variation of DOM molecules. More importantly, according to the NOSC value, the ratio 0.5 case exhibited a significantly higher median (−0.263) than the other two cases (−0.553 and −0.379 for control and ratio 1 cases, respectively), implying that molecules formed by the specific ozone dose of 0.5 were more bioavailable since the NOSC value reflected the bioavailability of molecules. (42,46) On the basis of the aforementioned findings, we constructed a series of membrane filtration systems fed with the ozonized waters to investigate the biofilm formation and associated mechanisms, which warrant special attention for the long-term membrane operation in water treatment.
关于计算出的AI值，比率0.5的中位数（0.179）明显低于其他臭氧处理的中位数（对照组和比率1病例分别为0.313和0.281），这进一步表明了0.5时的特定臭氧剂量在DOM分子变化中的过渡作用。更重要的是，根据NOSC值，比率0.5的中位数（-0.263）明显高于其他两种情况（对照组和比率1病例的中位数分别为-0.553和-0.379），这意味着由0.5的特定臭氧剂量形成的分子具有更高的生物利用度，因为NOSC值反映了分子的生物利用度。（42,46）基于上述研究结果，我们构建了一系列以臭氧水为食源的膜过滤系统，以研究生物膜的形成及其相关机制，这对于水处理中膜的长期运行需要特别关注。
关于计算出的AI值，比率0.5的中位数（0.179）明显低于其他臭氧处理的中位数（对照组和比率1病例分别为0.313和0.281），这进一步表明了0.5时的特定臭氧剂量在DOM分子变化中的过渡作用。更重要的是，根据NOSC值，比率0.5的中位数（-0.263）明显高于其他两种情况（对照组和比率1病例的中位数分别为-0.553和-0.379），这意味着由0.5的特定臭氧剂量形成的分子具有更高的生物利用度，因为NOSC值反映了分子的生物利用度。（42,46）基于上述研究结果，我们构建了一系列以臭氧水为食源的膜过滤系统，以研究生物膜的形成及其相关机制，这对于水处理中膜的长期运行需要特别关注。
3.2. Shifts in Biofilm Bacterial Community
3.2. 生物膜细菌群落的变化
As revealed by high-throughput sequencing data (Figure 2), the biofilm bacterial composition varied as a function of specific ozone dose. Specifically, a total of 49 amplicon sequence variants (ASVs) were presented in all the biofilms, and the number of shared ASVs was 44 for the ratio 0.5 and ratio 1 biofilms, which was larger than that for the control/ratio 0.5 and control/ratio 1 biofilms (both 27 ASVs; Figure 2A). This implied the commonness and otherness of the bacterial species in the course of ozonation. In addition, it was noted that the ASVs unique to the control biofilm possessed the highest number of 229, as compared to the number of 105 and 57 for the ratio 0.5 and ratio 1 biofilms, respectively. That is, some of the bacterial species were maladaptive to the increased specific ozone dose and disappeared or died. For detailed information about the bacteria, the bacterial community was taxonomically unveiled. The phylum Proteobacteria consistently occurred in very high members in all the biofilms, while differences can be seen clearly in Figure 2B. For the control biofilm, the occupied percentage was 52.9% but reached 67.9% in the biofilm of ratio 1. Consistent with this, Ribeirinho-Soares et al. discovered that ozonation promoted alteration of the microbial community, leading to the predominance of Proteobacteria. (47) The flagella were reported to assist Proteobacteria in resisting unfavorable external conditions (e.g., ozonation) by means of movement and thus contributed to the proliferation of Proteobacteria, which may be the reason for the increase in the relative abundance. (48) Furthermore, with regard to the sub-dominant phylum Planctomycetes, the increase in specific ozone dose varied its proportion from ∼7.6% (control) to ∼25.3% (ratio 0.5) and ∼19.6% (ratio 1), reflecting the influence of ozone treatment on the bacterial community. (49) It was discovered that the members of Planctomycetes played an important role in degrading DOM and the different proportion of Planctomycetes may lead to the formation of varying biofilms, which will be evaluated in the following discussion. (50)
正如高通量测序数据（图2）所揭示的那样，生物膜细菌组成随特定臭氧剂量的变化而变化。具体而言，所有生物膜共呈现49个扩增子序列变异（ASV），比值0.5和比值1的生物膜共用ASV数为44个，大于对照/比值0.5和对照/比值1生物膜（均为27个ASV;图2A）。这意味着细菌物种在臭氧化过程中的共同性和他者性。此外，值得注意的是，对照生物膜特有的ASV数量最多，为229，而比例为0.5和比例1的生物膜分别为105和57。也就是说，一些细菌物种对增加的特定臭氧剂量不适应，消失或死亡。有关细菌的详细信息，细菌群落在分类学上被揭示出来。变形菌门在所有生物膜中始终出现在非常高的成员中，而在图2B中可以清楚地看到差异。对于对照生物膜，占率为52.9%，但在比率为1的生物膜中达到67.9%。与此一致，Ribeirinho-Soares等人发现臭氧作用促进了微生物群落的改变，导致变形菌占主导地位。（47）据报道，鞭毛有助于变形菌通过运动抵抗不利的外部条件（例如臭氧化），从而促进变形菌的增殖，这可能是相对丰度增加的原因。（48）此外，对于亚优势门浮游菌门，特定臭氧剂量的增加比例从∼7.6%（对照）到∼25.3%（比率0.5）和∼19。6%（比率1），反映了臭氧处理对细菌群落的影响。（49）研究发现，浮游菌的成员在DOM降解中起着重要作用，浮游菌的不同比例可能导致不同生物膜的形成，这将在下文的讨论中进行评估。 (50)
正如高通量测序数据（图2）所揭示的那样，生物膜细菌组成随特定臭氧剂量的变化而变化。具体而言，所有生物膜共呈现49个扩增子序列变异（ASV），比值0.5和比值1的生物膜共用ASV数为44个，大于对照/比值0.5和对照/比值1生物膜（均为27个ASV;图2A）。这意味着细菌物种在臭氧化过程中的共同性和他者性。此外，值得注意的是，对照生物膜特有的ASV数量最多，为229，而比例为0.5和比例1的生物膜分别为105和57。也就是说，一些细菌物种对增加的特定臭氧剂量不适应，消失或死亡。有关细菌的详细信息，细菌群落在分类学上被揭示出来。变形菌门在所有生物膜中始终出现在非常高的成员中，而在图2B中可以清楚地看到差异。对于对照生物膜，占率为52.9%，但在比率为1的生物膜中达到67.9%。与此一致，Ribeirinho-Soares等人发现臭氧作用促进了微生物群落的改变，导致变形菌占主导地位。（47）据报道，鞭毛有助于变形菌通过运动抵抗不利的外部条件（例如臭氧化），从而促进变形菌的增殖，这可能是相对丰度增加的原因。（48）此外，对于亚优势门浮游菌门，特定臭氧剂量的增加比例从∼7.6%（对照）到∼25.3%（比率0.5）和∼19。6%（比率1），反映了臭氧处理对细菌群落的影响。（49）研究发现，浮游菌的成员在DOM降解中起着重要作用，浮游菌的不同比例可能导致不同生物膜的形成，这将在下文的讨论中进行评估。 (50)
Figure 2 图2
Figure 2. Compositional and diversity patterns of biofilm microbial consortium. (A) Upset plot of the average number of bacterial ASVs shared in the control, ratio 0.5, and ratio 1 biofilms. (B,C) Average relative abundance of bacterial taxa at phylum and genus levels, respectively. (D–G) Shannon, Simpson, Chao 1, and Pielou evenness indexes of the biofilm microbial consortium, respectively. (H) PCoA plot of the biofilm bacterial communities based on the Bray–Curtis distance matrix. (I) Bray–Curtis dissimilarity of bacterial community across different biofilms. Significant differences were investigated using the Kruskal–Wallis test. The marks a, b, and c in bold indicate statistical significance at P < 0.05.
图2.生物膜微生物联盟的组成和多样性模式。（A） 对照中共享的细菌 ASV 平均数量的扰动图，比率 0.5 和比率 1 生物膜。（乙、丙）细菌类群在门和属水平上的平均相对丰度。（D-G）Shannon、Simpson、Chao 1 和 Pielou 分别是生物膜微生物联盟的均匀度指数。（H） 基于Bray-Curtis距离矩阵的生物膜细菌群落PCoA图。（I）不同生物膜上细菌群落的Bray-Curtis差异。使用 Kruskal-Wallis 检验研究了显着差异。粗体标记 a、b 和 c 表示 P < 0.05 时的统计学显著性。
To provide further insights into the shifts in the community, we analyzed the microorganisms at the genus level. As demonstrated by Figure 2C, genera Gemmata and Bradythizobium dominated the control biofilm and the relative abundance outnumbered 25%. When the specific ozone dose increased to 0.5, the most abundant species shifted to Gemmata, reaching an average proportion of 42.3%. It should be noted that when the specific ozone dose increased to one, the opportunistic pathogen, Legionella, occurred in ∼40.0% abundance, which was much greater than that for the control (∼4.9%) and ratio of 0.5 biofilms (∼8.4%). The genus Legionella is a Gram-negative facultative intracellular bacterium widely distributed in the natural environment as well as in engineering water systems. (51) It was reported that biofilm was considered as one of the main reservoirs of Legionella, (52) where protozoa represented a key factor on the survival of Legionella by providing amino acids for intracellular growth and acting as shelter against hostile environmental conditions and disinfection agents. (53) Importantly, Legionella is able to regrow after exposure to ozone in the absence of residual ozone, (54) which may explain why Legionella occupied a high relative abundance in the biofilms formed with ozonized water.
为了进一步了解群落的变化，我们在属水平上分析了微生物。如图2C所示，Gemmata属和Bradythizobium属在对照生物膜中占主导地位，相对丰度超过25%。当臭氧比剂量增加到0.5时，最丰富的物种转移到Gemmata，平均比例达到42.3%。应该注意的是，当特定臭氧剂量增加到1时，机会性病原体军团菌的丰度约为40.0%，远高于对照组（∼4.9%）和0.5个生物膜的比例（∼8.4%）。军团菌属是一种革兰氏阴性兼性细胞内细菌，广泛分布在自然环境和工程水系统中。（51）据报道，生物膜被认为是军团菌的主要宿主之一，（52）其中原生动物通过为细胞内生长提供氨基酸并作为抵御恶劣环境条件和消毒剂的庇护所，是军团菌生存的关键因素。（53）重要的是，军团菌在没有残留臭氧的情况下暴露于臭氧后能够再生，（54）这可以解释为什么军团菌在臭氧水形成的生物膜中占据了较高的相对丰度。
为了进一步了解群落的变化，我们在属水平上分析了微生物。如图2C所示，Gemmata属和Bradythizobium属在对照生物膜中占主导地位，相对丰度超过25%。当臭氧比剂量增加到0.5时，最丰富的物种转移到Gemmata，平均比例达到42.3%。应该注意的是，当特定臭氧剂量增加到1时，机会性病原体军团菌的丰度约为40.0%，远高于对照组（∼4.9%）和0.5个生物膜的比例（∼8.4%）。军团菌属是一种革兰氏阴性兼性细胞内细菌，广泛分布在自然环境和工程水系统中。（51）据报道，生物膜被认为是军团菌的主要宿主之一，（52）其中原生动物通过为细胞内生长提供氨基酸并作为抵御恶劣环境条件和消毒剂的庇护所，是军团菌生存的关键因素。（53）重要的是，军团菌在没有残留臭氧的情况下暴露于臭氧后能够再生，（54）这可以解释为什么军团菌在臭氧水形成的生物膜中占据了较高的相对丰度。
To decipher the induced disparities in the diversity patterns of communities, attention was paid to biodiversity. As revealed by diversity indexes, such as the Shannon and Simpson indexes, the values significantly declined with the increase of specific ozone dose (Kruskal–Wallis test, P < 0.05; Figure 2D,E). Also, the richness and evenness decreased significantly in the course of increasing specific ozone dose, as witnessed by the declining trend of the Chao 1 (Kruskal–Wallis test, P < 0.05; Figure 2F) and Pielou evenness indexes (Kruskal–Wallis test, P < 0.05; Figure 2G). These implied that the higher specific ozone dose contributed to the lower biodiversity of microbial community and the findings by Gerrity et al. also supported this. (55)
为了破译群落多样性格局的诱发差异，人们关注了生物多样性。正如多样性指数（如Shannon指数和Simpson指数）所揭示的那样，随着特定臭氧剂量的增加，这些值显著下降（Kruskal-Wallis检验，P < 0.05;图2D，E）。此外，在增加特定臭氧剂量的过程中，丰富度和均匀度显著下降，正如Chao 1的下降趋势所证明的那样（Kruskal-Wallis检验，P < 0.05;图2F）和Pielou均匀度指数（Kruskal-Wallis检验，P < 0.05;图2G）。这些都表明，较高的特定臭氧剂量导致微生物群落的生物多样性较低，Gerrity等人的研究结果也支持了这一点。(55)
为了破译群落多样性格局的诱发差异，人们关注了生物多样性。正如多样性指数（如Shannon指数和Simpson指数）所揭示的那样，随着特定臭氧剂量的增加，这些值显著下降（Kruskal-Wallis检验，P < 0.05;图2D，E）。此外，在增加特定臭氧剂量的过程中，丰富度和均匀度显著下降，正如Chao 1的下降趋势所证明的那样（Kruskal-Wallis检验，P < 0.05;图2F）和Pielou均匀度指数（Kruskal-Wallis检验，P < 0.05;图2G）。这些都表明，较高的特定臭氧剂量导致微生物群落的生物多样性较低，Gerrity等人的研究结果也支持了这一点。(55)
In terms of community β-diversity, the PCoA plot based on the Bray–Curtis distance matrix revealed that the bacterial communities were clearly separated from each other under different treatments (Figure 2H), which further corroborated that the specific ozone dose affected the biofilm bacterial community. As quantified by Bray–Curtis dissimilarity, it was seen that the discrepancy between the control and ratio 1 communities was significantly high (Kruskal–Wallis test, P < 0.05), as evidenced by the greatest value (median ∼87.0%; Figure 2I). Comparatively, there was less difference between the control and ratio 0.5 bacterial communities (median ∼80.6%) and the Bray–Curtis dissimilarity was pronouncedly low for the group of ratio 0.5/ratio 1 (median ∼71.2%). Thus, the specific ozone dose played a substantial role in the alteration of the microbial community, and a larger differential resulted from the increase in the specific ozone dose. In contrast to the previous results for the molecular-level DOM, the turning point did not appear for the bacterial community. This indicated that the specific ozone dose had divergent influences on the water DOM and biofilm bacterial composition. While the DOM chemical composition affected the bacterial species less in comparison to the specific ozone dose, it may play a paramount role in biofilm accumulation. Therefore, the subsequent results were concerned with the properties of accumulated biofilms and the associated filtration performance.
在群落β多样性方面，基于Bray-Curtis距离矩阵的PCoA图显示，在不同处理下，细菌群落彼此分离明显（图2H），进一步证实了特定臭氧剂量对生物膜细菌群落的影响。通过 Bray-Curtis 差异量化，可以看出对照组和比率 1 群落之间的差异显著高（Kruskal-Wallis 检验，P < 0.05），最大值证明了这一点（中位数 ∼87.0%;图2I）。相比之下，对照组和比率 0.5 细菌群落之间的差异较小（中位数 ∼80.6%），比率 0.5/比率 1 组（中位数 ∼71.2%）的 Bray-Curtis 差异明显较低。因此，特定臭氧剂量在微生物群落的改变中起着重要作用，并且特定臭氧剂量的增加导致了更大的差异。与之前分子水平DOM的结果相比，细菌群落没有出现转折点。这表明特定臭氧剂量对水DOM和生物膜细菌组成有不同影响。虽然与特定臭氧剂量相比，DOM化学成分对细菌种类的影响较小，但它可能在生物膜积累中起着至关重要的作用。因此，随后的结果与积累的生物膜的性质和相关的过滤性能有关。
在群落β多样性方面，基于Bray-Curtis距离矩阵的PCoA图显示，在不同处理下，细菌群落彼此分离明显（图2H），进一步证实了特定臭氧剂量对生物膜细菌群落的影响。通过 Bray-Curtis 差异量化，可以看出对照组和比率 1 群落之间的差异显著高（Kruskal-Wallis 检验，P < 0.05），最大值证明了这一点（中位数 ∼87.0%;图2I）。相比之下，对照组和比率 0.5 细菌群落之间的差异较小（中位数 ∼80.6%），比率 0.5/比率 1 组（中位数 ∼71.2%）的 Bray-Curtis 差异明显较低。因此，特定臭氧剂量在微生物群落的改变中起着重要作用，并且特定臭氧剂量的增加导致了更大的差异。与之前分子水平DOM的结果相比，细菌群落没有出现转折点。这表明特定臭氧剂量对水DOM和生物膜细菌组成有不同影响。虽然与特定臭氧剂量相比，DOM化学成分对细菌种类的影响较小，但它可能在生物膜积累中起着至关重要的作用。因此，随后的结果与积累的生物膜的性质和相关的过滤性能有关。
3.3. Morphological Structure of Biofilm
3.3. 生物膜的形态结构
According to the images captured by SEM in the cross section, discrepancies were evident in the thickness of different biofilms (Figure 3A). Unexpectedly, the ratio 0.5 biofilm possessed the least thickness, yielding 70.7 ± 2.8 μm, which was only 14.2% of the control biofilm (496.2 ± 44.9 μm). In contrast, when the specific ozone dose increased to one (ratio 1), the biofilm thickness was approximately 227.9 μm, 3.2 times that of the ratio 0.5 biofilm, but only 45.9% of the control biofilm. This showed that ozonation of the feedwater indeed decreased the thickness of the biofilm, but the decline was not proportional to the increase of specific ozone dose. This discrepancy was probably caused by the different bioavailability of the feedwater DOM (Figure 1I) and the ability of intercepted bacteria to secrete EPS, wherein the former may play a more significant role and could be interpreted as follows. As deciphered on the molecular level, the DOM molecules formed under a specific ozone dose of 0.5 were more bioavailable in comparison to the other treatments (Figure 1I), contributing to the reduced accumulation in the biofilm. Apart from the differences in biofilm thickness, all the biofilms demonstrated network structures with a variety of pore sizes when viewed from the top (Figure 3B), which was unrelated to the specific ozone dose employed, suggesting the commonness of the biofilm in physical structure. (1,26,56,57)
根据SEM在横截面上捕获的图像，不同生物膜的厚度存在明显差异（图3A）。出乎意料的是，比例为0.5的生物膜具有最小的厚度，产生70.7±2.8μm，仅为对照生物膜（496.2±44.9μm）的14.2%。相反，当特定臭氧剂量增加到1（比率1）时，生物膜厚度约为227.9μm，是比率0.5生物膜的3.2倍，但仅为对照生物膜的45.9%。这表明给水的臭氧确实减少了生物膜的厚度，但这种下降与特定臭氧剂量的增加不成比例。这种差异可能是由于给水DOM的生物利用度不同（图1I）和截获的细菌分泌EPS的能力造成的，其中前者可能起着更重要的作用，可以解释如下。正如在分子水平上所破译的那样，与其他处理相比，在0.5的特定臭氧剂量下形成的DOM分子具有更高的生物利用度（图1I），有助于减少生物膜中的积累。除了生物膜厚度的差异外，从顶部观察时，所有生物膜都显示出具有不同孔径的网络结构（图3B），这与所采用的特定臭氧剂量无关，表明生物膜在物理结构中的共性。(1,26,56,57)
根据SEM在横截面上捕获的图像，不同生物膜的厚度存在明显差异（图3A）。出乎意料的是，比例为0.5的生物膜具有最小的厚度，产生70.7±2.8μm，仅为对照生物膜（496.2±44.9μm）的14.2%。相反，当特定臭氧剂量增加到1（比率1）时，生物膜厚度约为227.9μm，是比率0.5生物膜的3.2倍，但仅为对照生物膜的45.9%。这表明给水的臭氧确实减少了生物膜的厚度，但这种下降与特定臭氧剂量的增加不成比例。这种差异可能是由于给水DOM的生物利用度不同（图1I）和截获的细菌分泌EPS的能力造成的，其中前者可能起着更重要的作用，可以解释如下。正如在分子水平上所破译的那样，与其他处理相比，在0.5的特定臭氧剂量下形成的DOM分子具有更高的生物利用度（图1I），有助于减少生物膜中的积累。除了生物膜厚度的差异外，从顶部观察时，所有生物膜都显示出具有不同孔径的网络结构（图3B），这与所采用的特定臭氧剂量无关，表明生物膜在物理结构中的共性。(1,26,56,57)
Figure 3 图3
Figure 3. Morphological and chemical structure of biofilms. (A,B) SEM images of biofilms captured in cross-section and top surface, respectively. (C,D) XPS spectra of the biofilms based on elements C and O, respectively.
图3.生物膜的形态和化学结构。（甲、乙）分别在横截面和顶面捕获的生物膜的SEM图像。（C，D）分别基于元素 C 和 O 的生物膜的 XPS 光谱。
With regard to the chemical structure of the biofilms, the XPS full spectra revealed that elements C and O occurred in comparatively high intensity (Supporting Information Figure S3) and accordingly, we deciphered these elements with fine spectra (Figure 3C,D). As demonstrated in Figure 3C, the XPS spectra of biofilms showed three types of C peaks, being C–C (284.8 eV), C–O–C (286.6 eV), and O–CO (288.1, 288.3, and 288.4 eV), respectively. (58) While the species of C peaks were the same, there were discernible differences in terms of proportion (Figure 3C). For the C–C bond, the area percent increased from 43.0% (control) to 64.7% (ratio 0.5) and then decreased to 29.6% (ratio 1). In contrast, the C–O–C and the O–CO bonds showed a reverse variation trend. The area percents of C–O–C and O–CO bonds in the control biofilm were 41.3 and 15.7%, respectively. Then, they declined to 27.8 and 7.5% for the ratio 0.5 biofilm, but thereafter, increased to 49.9 and 20.5% as the specific ozone dose increased to one (Figure 3C). With respect to the XPS spectra of element O, the peaks (532.1/532.2 and 532.9/533.0 eV) assigned to CO and C–O species (Figure 3D) (58) presented a different variation trend with the increase of specific ozone dose. The C–O species had a tendency to decrease (from 49.5 to 44.6%) and then increase (73.4%) in the course of increasing specific ozone dose, in concordance with that for the C–O–C species deciphered from element C (Figure 3C). These observations provided further evidence to explain the turning point of the specific ozone dose at 0.5 and implied that the molecular-level DOM composition of the feedwater could exert an influence on the biofilm chemical bonds.
关于生物膜的化学结构，XPS全光谱显示元素C和O以相对较高的强度出现（支持信息图S3），因此，我们用精细光谱破译了这些元素（图3C，D）。如图3C所示，生物膜的XPS谱图显示了三种类型的C峰，分别是C-C（284.8 eV）、C-O-C（286.6 eV）和O-CO（288.1、288.3和288.4 eV）。（58）虽然C峰的种类相同，但在比例方面存在明显差异（图3C）。对于C-C键，面积百分比从43.0%（对照）增加到64.7%（比率0.5），然后下降到29.6%（比率1）。相比之下，C-O-C键和O-CO键呈现出相反的变化趋势。对照生物膜中C-O-C和O-CO键的面积百分比分别为41.3%和15.7%。然后，对于0.5生物膜的比率，它们下降到27.8%和7.5%，但此后，随着特定臭氧剂量增加到1，它们增加到49.9%和20.5%（图3C）。关于元素O的XPS光谱，分配给CO和C-O物种的峰（532.1/532.2和532.9/533.0 eV）（图3D）（58）随着特定臭氧剂量的增加而呈现出不同的变化趋势。在增加特定臭氧剂量的过程中，C-O物种有减少（从49.5%到44.6%）然后增加（73.4%）的趋势，这与从C元素中破译的C-O-C物种一致（图3C）。这些观察结果为解释0.5时特定臭氧剂量的转折点提供了进一步的证据，并暗示给水的分子水平DOM组成可能对生物膜化学键产生影响。
关于生物膜的化学结构，XPS全光谱显示元素C和O以相对较高的强度出现（支持信息图S3），因此，我们用精细光谱破译了这些元素（图3C，D）。如图3C所示，生物膜的XPS谱图显示了三种类型的C峰，分别是C-C（284.8 eV）、C-O-C（286.6 eV）和O-CO（288.1、288.3和288.4 eV）。（58）虽然C峰的种类相同，但在比例方面存在明显差异（图3C）。对于C-C键，面积百分比从43.0%（对照）增加到64.7%（比率0.5），然后下降到29.6%（比率1）。相比之下，C-O-C键和O-CO键呈现出相反的变化趋势。对照生物膜中C-O-C和O-CO键的面积百分比分别为41.3%和15.7%。然后，对于0.5生物膜的比率，它们下降到27.8%和7.5%，但此后，随着特定臭氧剂量增加到1，它们增加到49.9%和20.5%（图3C）。关于元素O的XPS光谱，分配给CO和C-O物种的峰（532.1/532.2和532.9/533.0 eV）（图3D）（58）随着特定臭氧剂量的增加而呈现出不同的变化趋势。在增加特定臭氧剂量的过程中，C-O物种有减少（从49.5%到44.6%）然后增加（73.4%）的趋势，这与从C元素中破译的C-O-C物种一致（图3C）。这些观察结果为解释0.5时特定臭氧剂量的转折点提供了进一步的证据，并暗示给水的分子水平DOM组成可能对生物膜化学键产生影响。
3.4. Physicochemical Property of Biofilm Matrix
3.4. 生物膜基质的理化性质
As shown by fluorescence spectra (Figure 4A), two main peaks appeared for all the biofilm DOM, tyrosine- and tryptophan-like substances in regions I and IV, respectively. According to the demonstrated colors, the ratio 0.5 biofilm exhibited a discernably lower fluorescence intensity in comparison to that for the ratio 1 and control biofilms, which was inversely proportional to the bioavailability of feedwater DOM. That is, the greater the bioavailability of feedwater DOM the less fluorescent the DOM accumulated in the biofilm. In terms of the functional groups in the biofilm matrix, the representative FTIR spectra indicated abundant peaks with varied absorption intensities, such as −OH–, CO, amide I, amide II, amide III, C–O–C, and C–O (Figure 4B). Although there was only a little difference in the intensity for different biofilms, the absorption of −OH– was obviously strong, which was beneficial for the biofilm to remove undesired pollutants from the influent flow.
如荧光光谱所示（图4A），所有生物膜DOM，酪氨酸和色氨酸样物质分别在I区和IV区出现两个主峰。根据所展示的颜色，与比例 1 和对照生物膜相比，比例 0.5 生物膜的荧光强度明显较低，这与给水 DOM 的生物利用度成反比。也就是说，给水DOM的生物利用度越高，DOM在生物膜中积累的荧光就越少。就生物膜基质中的官能团而言，具有代表性的FTIR光谱显示出具有不同吸收强度的丰富峰，例如-OH–，CO，酰胺I，酰胺II，酰胺III，C-O-C和C-O（图4B）。虽然不同生物膜的强度差异不大，但−OH-的吸收明显较强，有利于生物膜去除进水流中不需要的污染物。
如荧光光谱所示（图4A），所有生物膜DOM，酪氨酸和色氨酸样物质分别在I区和IV区出现两个主峰。根据所展示的颜色，与比例 1 和对照生物膜相比，比例 0.5 生物膜的荧光强度明显较低，这与给水 DOM 的生物利用度成反比。也就是说，给水DOM的生物利用度越高，DOM在生物膜中积累的荧光就越少。就生物膜基质中的官能团而言，具有代表性的FTIR光谱显示出具有不同吸收强度的丰富峰，例如-OH–，CO，酰胺I，酰胺II，酰胺III，C-O-C和C-O（图4B）。虽然不同生物膜的强度差异不大，但−OH-的吸收明显较强，有利于生物膜去除进水流中不需要的污染物。
Figure 4 图4
Figure 4. Physicochemical properties of the biofilm matrix. (A) Representative fluorescence spectra of the DOM extracted in the biofilm matrix with phosphate buffer solution. (B) Representative FTIR spectra. (C) Representative optical micrographs and the corresponding surface roughness. (D) Concentrations of polysaccharides and proteins. (E) Representative Raman spectra. Significant differences were assessed by the Kruskal–Wallis test and * represents P < 0.05.
图4.生物膜基质的物理化学性质。（A）用磷酸盐缓冲溶液在生物膜基质中提取的DOM的代表性荧光光谱。（B） 具有代表性的傅里叶变换红外光谱。（C）具有代表性的光学显微照片和相应的表面粗糙度。（D） 多糖和蛋白质的浓度。（E） 具有代表性的拉曼光谱。通过 Kruskal-Wallis 检验评估显著差异，* 表示 P < 0.05。
With regard to surface morphology, divergent aggregation states of the biofilm matrix were induced by the varying specific ozone dose as revealed by InfiniteFocus G5, which tended to be sparser with the increase of the specific ozone dose (Figure 4C). Meanwhile, the surface roughness was reduced, as indicated by the Sq value (Figure 4C and Supporting Information Table S2), giving values in the sequence of, the control (2.516 μm) > ratio 0.5 (1.540 μm) > ratio 1 (0.873 μm), which was suspected to be the co-effect generated by the bacteria and DOM. Interestingly, according to the quantified results, the ratio 1 sample yielded about 2.5 times greater concentrations of polysaccharides (173.52 ± 3.77 μg·cm–2) and proteins (30.41 ± 1.53 μg·cm–2) than those for the ratio 0.5 sample (50.60 ± 2.22 and 8.05 ± 0.92 μg·cm–2 for polysaccharides and proteins, respectively), in line with the observed greater biofilm thickness (Figure 3A) and stronger fluorescence intensity (Figure 4A). This further implied the role of the bioavailability of the feedwater DOM in the influence of accumulated matter.
在表面形态方面，生物膜基质的不同聚集状态是由InfiniteFocus G5揭示的比臭氧剂量的变化引起的，随着比臭氧剂量的增加，生物膜基质趋于稀疏（图4C）。同时，表面粗糙度降低，如Sq值（图4C和支持信息表S2）所示，按对照（2.516μm）>比0.5（1.540μm）>比1（0.873μm）的顺序给出值，怀疑这是细菌和DOM产生的共同效应。 有趣的是，根据量化结果， 比例1样品的多糖浓度（173.52 ± 3.77 μg·cm –2 ）和蛋白质（30.41 ± 1.53 μg·cm –2 ）的浓度是比例0.5样品（多糖和蛋白质分别为50.60±2.22和8.05 ± 0.92 μg·cm –2 ）的2.5倍，与观察到的更大的生物膜厚度（图3A）和更强的荧光强度（图4A）一致。这进一步暗示了给水DOM的生物利用度在累积物质的影响中的作用。
在表面形态方面，生物膜基质的不同聚集状态是由InfiniteFocus G5揭示的比臭氧剂量的变化引起的，随着比臭氧剂量的增加，生物膜基质趋于稀疏（图4C）。同时，表面粗糙度降低，如Sq值（图4C和支持信息表S2）所示，按对照（2.516μm）>比0.5（1.540μm）>比1（0.873μm）的顺序给出值，怀疑这是细菌和DOM产生的共同效应。 有趣的是，根据量化结果， 比例1样品的多糖浓度（173.52 ± 3.77 μg·cm –2 ）和蛋白质（30.41 ± 1.53 μg·cm –2 ）的浓度是比例0.5样品（多糖和蛋白质分别为50.60±2.22和8.05 ± 0.92 μg·cm –2 ）的2.5倍，与观察到的更大的生物膜厚度（图3A）和更强的荧光强度（图4A）一致。这进一步暗示了给水DOM的生物利用度在累积物质的影响中的作用。
The representative Raman spectra displayed three major peaks in all the biofilms at 1004 (α), 1155 (β), and 1512 cm–1 (γ), which were associated with the vibrations of P–O–P, C–O–C, and −COO–, respectively, (59) providing valuable complementary information to the FTIR spectra. The P–O–P groups constitute the phosphate backbone of the DNA molecules and the presence of −COO– groups implies a connection between neighboring anionic polymers through electrostatic interactions. (59,60) In addition, the Raman activity of the control biofilm was evidently the highest, followed by the ratio 1 and ratio 0.5 biofilms, which also indicated the turning point of the specific ozone dose at 0.5.
具有代表性的拉曼光谱在所有生物膜中分别在1004（α）、1155（β）和1512 cm –1 （γ）处显示出三个主要峰，分别与P-O-P、C-O-C和-COO – 的振动有关（59），为FTIR光谱提供了有价值的补充信息。P-O-P基团构成DNA分子的磷酸盐骨架，−COO – 基团的存在意味着相邻阴离子聚合物之间通过静电相互作用进行连接。（59,60）此外，对照生物膜的拉曼活性明显最高，其次是比值1和比值0.5的生物膜，这也表明比臭氧剂量的转折点为0.5。
具有代表性的拉曼光谱在所有生物膜中分别在1004（α）、1155（β）和1512 cm –1 （γ）处显示出三个主要峰，分别与P-O-P、C-O-C和-COO – 的振动有关（59），为FTIR光谱提供了有价值的补充信息。P-O-P基团构成DNA分子的磷酸盐骨架，−COO – 基团的存在意味着相邻阴离子聚合物之间通过静电相互作用进行连接。（59,60）此外，对照生物膜的拉曼活性明显最高，其次是比值1和比值0.5的生物膜，这也表明比臭氧剂量的转折点为0.5。
Collectively, the detailed investigation of the biofilm matrix properties provided further information about the role of specific ozone dose in biofilm formation and, moreover, the multifaceted features of the biofilm were found to be mutually corroborated. Therein, the feedwater DOM and biofilm bacteria jointly acted on the formation of biofilm, but their respective contribution was difficult to ascertain due to the experimental limitations.
总的来说，对生物膜基质特性的详细研究提供了关于特定臭氧剂量在生物膜形成中的作用的进一步信息，此外，生物膜的多方面特征被发现是相互印证的。其中，给水DOM和生物膜细菌共同作用于生物膜的形成，但由于实验的局限性，它们各自的贡献难以确定。
总的来说，对生物膜基质特性的详细研究提供了关于特定臭氧剂量在生物膜形成中的作用的进一步信息，此外，生物膜的多方面特征被发现是相互印证的。其中，给水DOM和生物膜细菌共同作用于生物膜的形成，但由于实验的局限性，它们各自的贡献难以确定。
3.5. Filtration Performance of Membrane System
3.5. 膜系统的过滤性能
The experiments showed that all of the filtration systems displayed excellent removal performance of fluorescent substances, especially tyrosine- and tryptophan-like substances in regions I and IV, respectively (Figure 5A). It should be noted that the effluent of the ratio 1 system presented an extremely low fluorescence intensity, which was around zero R.U. This implied that a specific ozone dose of 1 was sufficient to produce a high-quality effluent and that there would be no significant benefit in increasing the specific ozone dose further, which is an important factor for moderating costs in practical applications.
实验表明，所有过滤系统均表现出优异的荧光物质去除性能，尤其是I区和IV区的酪氨酸和色氨酸样物质（图5A）。应该注意的是，比率1系统的流出物呈现出极低的荧光强度，约为零R.U。这意味着1的特定臭氧剂量足以产生高质量的流出物，而进一步增加特定臭氧剂量不会有显着的好处，这是在实际应用中降低成本的重要因素。
实验表明，所有过滤系统均表现出优异的荧光物质去除性能，尤其是I区和IV区的酪氨酸和色氨酸样物质（图5A）。应该注意的是，比率1系统的流出物呈现出极低的荧光强度，约为零R.U。这意味着1的特定臭氧剂量足以产生高质量的流出物，而进一步增加特定臭氧剂量不会有显着的好处，这是在实际应用中降低成本的重要因素。
Figure 5 图5
Figure 5. Filtration performance of membrane systems. (A) Representative fluorescence spectra of DOM in the influents and effluents of membrane filtration systems. (B) Regional removal rate of fluorescence intensity by the membrane filtration systems. (C) Apparent molecular weight distribution profile of the DOM in the influents and effluents. (D) Hydraulic resistance of the membrane system in the course of filtration.
图5.膜系统的过滤性能。（A）DOM在膜过滤系统进水和出水中的代表性荧光光谱。（B）膜过滤系统对荧光强度的区域去除率。（C） DOM在进水和出水中的表观分子量分布曲线。（D）过滤过程中膜系统的水力阻力。
Regionally, according to the data in Figure 5B, the ratio 1 filtration system exhibited the best performance in removing substances in regions I, II, IV, and V, yielding 64.9 ± 6.6, 43.6 ± 7.0, 59.4 ± 9.0, and 12.6 ± 1.0%, respectively. This could be ascribed to the comparatively greater thickness of biofilm (in comparison to the ratio 0.5 sample) and, more importantly, the low richness of the microbial consortium, since abundant microbes would secrete amounts of fluorescent substances. Interestingly, in terms of fulvic acid- (region III) and humic acid-like substances (region V), the removal rate presented a trend consistent with that of biofilm thickness, meaning that the thickness of the biofilm played an important role in removing these two kinds of substances.
从区域来看，根据图5B中的数据，比率1过滤系统在去除I、II、IV和V区域的物质方面表现最佳，分别产生64.9%±6.6%、43.6±7.0%、59.4±9.0%和12.6%±1.0%。这可能归因于生物膜的厚度相对较大（与0.5样品的比例相比），更重要的是，微生物联盟的丰富度较低，因为丰富的微生物会分泌大量的荧光物质。有趣的是，在富里酸（III区）和腐殖酸样物质（V区）方面，去除率呈现出与生物膜厚度一致的趋势，这意味着生物膜的厚度在去除这两种物质中起着重要作用。
从区域来看，根据图5B中的数据，比率1过滤系统在去除I、II、IV和V区域的物质方面表现最佳，分别产生64.9%±6.6%、43.6±7.0%、59.4±9.0%和12.6%±1.0%。这可能归因于生物膜的厚度相对较大（与0.5样品的比例相比），更重要的是，微生物联盟的丰富度较低，因为丰富的微生物会分泌大量的荧光物质。有趣的是，在富里酸（III区）和腐殖酸样物质（V区）方面，去除率呈现出与生物膜厚度一致的趋势，这意味着生物膜的厚度在去除这两种物质中起着重要作用。
From the perspective of apparent molecular weight (Figure 5C), ozonation effectively lowered the intensity of substances ranging from 600 to 10,000 Da, as demonstrated by the influent intensities of ratio 0.5 and ratio 1 samples. The intensity disparity was greater for the influent of control/ratio 0.5 samples than that of ratio 0.5/ratio 1 samples, suggesting that a further increase of specific ozone dose (>0.5) may lead to the limited improvement of removal efficiency.
从表观分子量（图5C）的角度来看，臭氧化有效地降低了600至10,000 Da范围内物质的强度，如比率0.5和比率1样品的进水强度所示。对照/比率0.5样品的进水强度差异大于比率0.5/比率1样品的强度差异，表明进一步增加比臭氧剂量（>0.5）可能导致去除效率的有限提高。
从表观分子量（图5C）的角度来看，臭氧化有效地降低了600至10,000 Da范围内物质的强度，如比率0.5和比率1样品的进水强度所示。对照/比率0.5样品的进水强度差异大于比率0.5/比率1样品的强度差异，表明进一步增加比臭氧剂量（>0.5）可能导致去除效率的有限提高。
Furthermore, the hydraulic resistance was investigated to evaluate the membrane filtration efficiency. As a function of filtration time, the control system always possessed the greatest hydraulic resistance, but the impact of ozone, while being beneficial in dramatically reducing the resistance, was unexpected, where the ratio 1 system exhibited a greater resistance value than the ratio 0.5 system. In the pseudo-stable period, the hydraulic resistance reached (2.32 ± 0.05) × 1012 m–1 and (5.16 ± 0.34) × 1012 m–1 for the ratio 0.5 and ratio 1 systems, respectively, which accounted for only about 13.5 and 30.0% percentage of the control system ((17.23 ± 1.21) × 1012 m–1). The corresponding permeate flux was 0.76 ± 0.05, 5.33 ± 0.10, and 2.49 ± 0.15 L·m–2·h–1 for the control, ratio 0.5, and ratio 1 filtration systems, respectively (Supporting Information Figure S4). These results have shown clearly that ozonation of the feedwater can improve membrane filtration efficiency, but the ozone dose needs to be optimized and excess ozonation avoided.
此外，还研究了水力阻力，以评估膜过滤效率。作为过滤时间的函数，控制系统始终具有最大的水力阻力，但臭氧的影响虽然有利于显着降低阻力，但出乎意料，其中比率 1 系统表现出比比率 0.5 系统更大的阻力值。在伪稳定期，比值0.5和比值1系统的水±力阻力分别达到10 12 12 m和（5.16 ± 0.34）××10 m –1 –1 和（5.16 0.34），仅占控制系统（（17.23 ± 1.21）×10 12 m –1 的13.5%和30.0%左右。对照、比率0.5和比率1过滤系统的渗透通量分别为0.76±0.05、5.33±0.10和2.49±0.15 L·m –2 ·h –1 （支持信息图S4）。这些结果清楚地表明，给水的臭氧化可以提高膜过滤效率，但臭氧剂量需要优化，避免过多的臭氧。
此外，还研究了水力阻力，以评估膜过滤效率。作为过滤时间的函数，控制系统始终具有最大的水力阻力，但臭氧的影响虽然有利于显着降低阻力，但出乎意料，其中比率 1 系统表现出比比率 0.5 系统更大的阻力值。在伪稳定期，比值0.5和比值1系统的水±力阻力分别达到10 12 12 m和（5.16 ± 0.34）××10 m –1 –1 和（5.16 0.34），仅占控制系统（（17.23 ± 1.21）×10 12 m –1 的13.5%和30.0%左右。对照、比率0.5和比率1过滤系统的渗透通量分别为0.76±0.05、5.33±0.10和2.49±0.15 L·m –2 ·h –1 （支持信息图S4）。这些结果清楚地表明，给水的臭氧化可以提高膜过滤效率，但臭氧剂量需要优化，避免过多的臭氧。
3.6. Synergistic Driving Mechanism of DOM and Biofilm Microbial Consortium on Membrane Filtration Efficiency
3.6. DOM和生物膜微生物联盟对膜过滤效率的协同驱动机制
3.6.1. Variation in DOM Molecules and Bacterial Community Triggered Discrepancy in Biofilm Morphology and Properties
3.6.1. DOM分子和细菌群落的变化引发了生物膜形态和性质的差异
The dosed ozone induced the transformation of molecular-level DOM in the feedwater, as deciphered by the ESI-FT-ICR data, but the variation in DOM molecules was contingent on the value of the specific ozone dose (Figure 1). The specific ozone dose of 0.5 was inferred to be a turning point in the DOM transformation, whereby the lowest AI value was obtained. Importantly, the molecules were highly bioavailable, indicating that they were readily accessible to the bacteria and thus easily degraded, which was beneficial in reducing the accumulation of water organic matter in the biofilm, as witnessed by the lower biofilm thickness (Figure 3A).
正如ESI-FT-ICR数据所揭示的那样，剂量臭氧诱导了给水中分子水平DOM的转变，但DOM分子的变化取决于特定臭氧剂量的值（图1）。据推测，0.5的比臭氧剂量是DOM转型的转折点，从而获得了最低的AI值。重要的是，这些分子具有很高的生物利用度，表明它们很容易被细菌接近，因此很容易降解，这有利于减少生物膜中水有机物的积累，正如较低的生物膜厚度所证明的那样（图3A）。
正如ESI-FT-ICR数据所揭示的那样，剂量臭氧诱导了给水中分子水平DOM的转变，但DOM分子的变化取决于特定臭氧剂量的值（图1）。据推测，0.5的比臭氧剂量是DOM转型的转折点，从而获得了最低的AI值。重要的是，这些分子具有很高的生物利用度，表明它们很容易被细菌接近，因此很容易降解，这有利于减少生物膜中水有机物的积累，正如较低的生物膜厚度所证明的那样（图3A）。
In addition, the biofilm microbial community also led to the variation of membrane filtration efficiency through secreting EPS. For the mature biofilms, the succession in the microbial community was influenced by both the specific ozone dose and influent DOM. Therein, the specific ozone dose played a selective role in the biofilm microbes due to the differential sensitivity and tolerance of microorganisms to the ozone dose. For example, Legionella was drastically stimulated by the high specific ozone dose of one (Figure 2C) as demonstrated in this study, and the microbial consortium shifted with the increase of the specific ozone dose (Figure 2B,C). The similarity between the ozonized and control bacterial communities decreased as the specific ozone dose increased, while the ratio 0.5/ratio 1 group exhibited a comparatively high similarity (Figure 2I), verifying the significant role of the specific ozone dose in altering the biofilm bacterial community. Consistent with this, Sun et al. also discovered that ozone oxidation affected the bacterial community in the biofilms. (22)
此外，生物膜微生物群落还通过分泌EPS导致膜过滤效率的变化。对于成熟的生物膜，微生物群落的演替受特定臭氧剂量和进水DOM的影响。 其中，由于微生物对臭氧剂量的敏感性和耐受性不同，特定臭氧剂量在生物膜微生物中起选择性作用。例如，如本研究所证明的那样，军团菌受到高比臭氧剂量的强烈刺激（图2C），微生物联盟随着特定臭氧剂量的增加而移动（图2B，C）。臭氧菌群落和对照细菌群落之间的相似性随着特定臭氧剂量的增加而降低，而比率0.5/比率1组表现出相对较高的相似性（图2I），验证了特定臭氧剂量在改变生物膜细菌群落方面的重要作用。与此一致，Sun等人还发现臭氧氧化影响了生物膜中的细菌群落。(22)
此外，生物膜微生物群落还通过分泌EPS导致膜过滤效率的变化。对于成熟的生物膜，微生物群落的演替受特定臭氧剂量和进水DOM的影响。 其中，由于微生物对臭氧剂量的敏感性和耐受性不同，特定臭氧剂量在生物膜微生物中起选择性作用。例如，如本研究所证明的那样，军团菌受到高比臭氧剂量的强烈刺激（图2C），微生物联盟随着特定臭氧剂量的增加而移动（图2B，C）。臭氧菌群落和对照细菌群落之间的相似性随着特定臭氧剂量的增加而降低，而比率0.5/比率1组表现出相对较高的相似性（图2I），验证了特定臭氧剂量在改变生物膜细菌群落方面的重要作用。与此一致，Sun等人还发现臭氧氧化影响了生物膜中的细菌群落。(22)
Meanwhile, the influent DOM provided substrates that acted as niches for the biofilm microbes, which could also affect the microbial species. (27,28) In this study, even though the biofilm microbial community presented an inconsistent variation with the influent DOM, owing to the weaker role of influent DOM in comparison to the specific ozone dose, the contribution of influent DOM to the biofilm microbial composition should not be neglected. As a consequence of the influences of the specific ozone dose and influent DOM, the biofilm microbial community varied, resulting in changes in the presence of EPS.
同时，进水DOM提供了基质，作为生物膜微生物的生态位，这也可能影响微生物物种。（27,28） 在这项研究中，尽管生物膜微生物群落与进水 DOM 呈现出不一致的变化，但由于进水 DOM 的作用与特定臭氧剂量相比较弱，但不应忽视进水 DOM 对生物膜微生物组成的贡献。由于特定臭氧剂量和进水DOM的影响，生物膜微生物群落各不相同，导致EPS的存在发生变化。
同时，进水DOM提供了基质，作为生物膜微生物的生态位，这也可能影响微生物物种。（27,28） 在这项研究中，尽管生物膜微生物群落与进水 DOM 呈现出不一致的变化，但由于进水 DOM 的作用与特定臭氧剂量相比较弱，但不应忽视进水 DOM 对生物膜微生物组成的贡献。由于特定臭氧剂量和进水DOM的影响，生物膜微生物群落各不相同，导致EPS的存在发生变化。
3.6.2. Induced Changes in Biofilm Drove Disparity in Membrane Filtration Performance
3.6.2. 生物膜的诱导变化导致膜过滤性能的差异
The generated variation in the accumulated influent DOM and EPS produced changes in the structures and properties of the biofilms, which further affected the membrane filtration efficiency. As revealed in this study, the ratio 0.5 filtration system demonstrated a reduced biofilm thickness (Figure 3A), weaker fluorescence intensity (Figure 4A), smaller concentrations of polysaccharides and proteins (Figure 4D), and lower Raman activity (Figure 4E). Accordingly, this resulted in a lower hydraulic resistance (Figure 5D) and higher permeate flux (Supporting Information Figure S4), as compared to the zero ozone and the higher (excessive) ratio 1 membrane filtration systems. The findings by Desmond et al. also supported this, revealing that the composition of EPS could determine the meso-scale physical structure of membrane biofilms and in turn its hydraulic resistance. (24)
累积进水DOM和EPS的变化导致生物膜的结构和性质发生变化，进一步影响了膜过滤效率。正如本研究所揭示的那样，比率为0.5的过滤系统显示出生物膜厚度减小（图3A），荧光强度减弱（图4A），多糖和蛋白质浓度降低（图4D）和拉曼活性降低（图4E）。因此，与零臭氧和较高（过量）比率 1 的膜过滤系统相比，这导致了较低的水力阻力（图 5D）和更高的渗透液通量（支持信息图 S4）。Desmond等人的研究结果也支持了这一点，揭示了EPS的组成可以决定膜生物膜的介观物理结构，进而决定其水力阻力。(24)
累积进水DOM和EPS的变化导致生物膜的结构和性质发生变化，进一步影响了膜过滤效率。正如本研究所揭示的那样，比率为0.5的过滤系统显示出生物膜厚度减小（图3A），荧光强度减弱（图4A），多糖和蛋白质浓度降低（图4D）和拉曼活性降低（图4E）。因此，与零臭氧和较高（过量）比率 1 的膜过滤系统相比，这导致了较低的水力阻力（图 5D）和更高的渗透液通量（支持信息图 S4）。Desmond等人的研究结果也支持了这一点，揭示了EPS的组成可以决定膜生物膜的介观物理结构，进而决定其水力阻力。(24)
Supporting Information 支持信息
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The Supporting Information includes 4 figures and 3 tables, which supplement the results in the manuscript. These comprise the following: schematic diagram of membrane filtration system (Figure S1), FT-ICR mass spectra of influent DOM in membrane filtration systems (Figure S2), XPS full spectra of biofilms (Figure S3), variation in permeate flux of membrane filtration systems in the course of each experiment (Figure S4), principal water quality parameters of surface water (Table S1), area percent of XPS spectral peaks (Table S2), and biofilm surface texture of roughness data set (Table S3) (PDF)
支持信息包括 4 个图表和 3 个表格，补充了手稿中的结果。这些包括以下内容：膜过滤系统的示意图（图S1），膜过滤系统中进水DOM的FT-ICR质谱图（图S2），生物膜的XPS全谱图（图S3），膜过滤系统在每个实验过程中渗透通量的变化（图S4），地表水的主要水质参数（表S1）， XPS光谱峰的面积百分比（表S2）和粗糙度数据集的生物膜表面纹理（表S3）（PDF）
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Author Information 作者信息
- Wenzheng Yu - State Key Laboratory of Environmental Aquatic Chemistry, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing 100085, China;
https://orcid.org/0000-0001-9776-8021;
俞文正 - 中国科学院生态环境科学研究中心，环境水产化学国家重点实验室，中国北京100085; https://orcid.org/0000-0001-9776-8021;电子邮件： wzyu@rcees.ac.cn
- Yongguan Zhu - State Key Laboratory of Urban and Regional Ecology, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing 100085, China;https://orcid.org/0000-0003-3861-8482
朱永冠 - 中国科学院生态环境研究中心城市与区域生态国家重点实验室， 北京100085; https://orcid.org/0000-0003-3861-8482
Dr. Li Zhang did the experiments; Dr. Li Zhang, Professor Nigel Graham, and Wenzheng Yu exchanged research ideas, discussed the work, and contributed to the interpretation of the results. Professor Yongguan Zhu was involved in the design of the experiment and discussed the results of the research. Professor Guibai Li, Professor Nigel Graham, and Wenzheng Yu made the final version of the manuscript.
张李博士做了实验;张力博士、奈杰尔·格雷厄姆教授和俞文正交流了研究思路，讨论了工作，并对结果的解释做出了贡献。朱永冠教授参与了实验的设计，并讨论了研究成果。李桂白教授、奈杰尔·格雷厄姆教授和俞文正制作了手稿的最终版本。
Acknowledgments 确认
This research was supported financially by the Beijing Natural Science Fund for Distinguished Young Scholars (Grant no. JQ21032) and the National Natural Science Foundation of China (Grant no. 52370184).
本研究由北京市自然科学杰出青年基金资助。JQ21032）和国家自然科学基金（批准号：52370184）。
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This article references 60 other publications.
本文引用了60篇其他出版物。
- 1Zhang, L.; Graham, N.; Kimura, K.; Li, G.; Yu, W. Targeting membrane fouling with low dose oxidant in drinking water treatment: Beneficial effect and biological mechanism. Water Res.IF 12.8SCIEJCI 2.15Q1环境科学与生态学1区Top2022, 209, 117953, DOI: 10.1016/j.watres.2021.117953 Google Scholar Google 学术搜索There is no corresponding record for this reference.
1张，L.;格雷厄姆，N.;木村，K.;李，G.;Yu， W.在饮用水处理中用低剂量氧化剂靶向膜污染：有益效果和生物学机制。水研究 2022， 209， 117953， DOI： 10.1016/j.watres.2021.117953 - 2Yu, W.; Graham, N. J. D. Application of Fe(II)/K2MnO4 as a pre-treatment for controlling UF membrane fouling in drinking water treatment. J. Membr. Sci.IF 9.5SCIEJCI 1.85Q1工程技术1区Top2015, 473, 283– 291, DOI: 10.1016/j.memsci.2014.08.060 Google Scholar Google 学术搜索2https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC2cXhs1KgurbE&md5=a0ae48469b5bd5de4e6fc9373ada59c5Application of Fe(II)/K2MnO4 as a pre-treatment for controlling UF membrane fouling in drinking water treatmentYu, Wenzheng; Graham, Nigel. J. D.Journal of Membrane Science (2015), 473 (), 283-291CODEN: JMESDO; ISSN:0376-7388. (Elsevier B.V.)This paper describes some results of mini-pilot-scale tests concerning the performance of K2MnO4 as a pre-treatment chem. prior to ultrafiltration. Manganate is an intermediate in the com. prepn. of permanganate and in aq. reactions MnO42- can act as both an oxidant and a coagulant/adsorbent arising from the formation of insol. MnO2. The combination of ferrous sulfate and manganate (Fe/Mn), offers a potentially cheaper and effective combination of pre-oxidant and coagulant compared to the chems. used currently in water treatment (e.g., ozone, Cl, ferric sulfate). In comparative tests with conventional ferric sulfate and using simulated raw water, the results showed that Fe/Mn pre-treatment substantially reduced membrane fouling in terms of the rate of trans-membrane pressure development (arising from both external and internal fouling). Fe/Mn pre-treatment was effective in reducing bacterial activity, changing the characteristics of org. matter and decreasing the prodn. of extracellular polymeric substances (EPS) by bacteria. The external fouling in this process was detd. by the EPS concn., and the internal fouling mainly detd. by the adsorption of lower MW org. matter to the membrane pores. Fe/Mn pre-treatment reduced the amts. of both types of fouling material within the cake layer and membrane pores in comparison to conventional pre-treatment with ferrous sulfate, most likely through the formation of solid-phase Fe(III) and MnO2 and by MnO42- oxidn., thereby leading to a substantial increase in membrane run time.
2余，W.;Graham， N. J. D.Fe（II）/K 2 MnO 4 作为预处理在饮用水处理中控制超滤膜污垢的应用。J.门布尔。Sci.2015， 473， 283– 291， DOI： 10.1016/j.memsci.2014.08.060 - 3Yu, W.; Xu, L.; Graham, N.; Qu, J. Pre-treatment for ultrafiltration: Effect of pre-chlorination on membrane fouling. Sci. Rep.IF 4.6SCIEJCI 1.06Q2综合性期刊2区2014, 4, 6513, DOI: 10.1038/srep06513 Google Scholar Google 学术搜索3https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC2MXksVWmsbo%253D&md5=315394adaa8ecb9b3fd01f3f45d8263aPre-treatment for ultrafiltration: effect of pre-chlorination on membrane foulingYu, Wenzheng; Xu, Lei; Graham, Nigel; Qu, JiuhuiScientific Reports (2014), 4 (), 6513CODEN: SRCEC3; ISSN:2045-2322. (Nature Publishing Group)Microbial effects are believed to be a major contributor to membrane fouling in drinking water treatment. Sodium hypochlorite (NaClO) is commonly applied in membrane cleaning, but its potential use as a pretreatment for controlling operational fouling has received little attention. In this study, the effect of adding a continuous low dose of NaClO (1 mg/l as active Cl) in combination with alum, before ultrafiltration, was compared with only alum as pretreatment. The results showed that the addn. of NaClO substantially reduced membrane fouling both in terms of the rate of TMP development and the properties of the membrane cake layer. Although the size of nano-scale primary coagulant flocs changed little by the addn. of NaClO, the cake layer on the membrane had a greater porosity and a substantially reduced thickness. NaClO was found to inactivate bacteria in the influent flow, which reduced both microbial proliferation and the prodn. of proteins and polysaccharides in the cake layer and contributed significantly to improving the overall ultrafiltration performance. NaClO dosing had no adverse impact on the formation of currently regulated disinfection byproduct compds. (THMs and HAAs).
3余，W.;徐，L.;格雷厄姆，N.;曲，J.超滤预处理：预氯化对膜结垢的影响。Sci. Rep.2014， 4， 6513， DOI： 10.1038/srep06513 - 4Liu, T.; Chen, Z.-L.; Yu, W.-Z.; You, S.-J. Characterization of organic membrane foulants in a submerged membrane bioreactor with pre-ozonation using three-dimensional excitation-emission matrix fluorescence spectroscopy. Water Res.IF 12.8SCIEJCI 2.15Q1环境科学与生态学1区Top2011, 45 (5), 2111– 2121, DOI: 10.1016/j.watres.2010.12.023 Google Scholar Google 学术搜索4https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC3MXitFaqurY%253D&md5=d8862c5f758d9b4d58f6d80045804e9dCharacterization of organic membrane foulants in a submerged membrane bioreactor with pre-ozonation using three-dimensional excitation-emission matrix fluorescence spectroscopyLiu, Ting; Chen, Zhong-lin; Yu, Wen-zheng; You, Shi-jieWater Research (2011), 45 (5), 2111-2121CODEN: WATRAG; ISSN:0043-1354. (Elsevier B.V.)This study focuses on org. membrane foulants in a submerged membrane bioreactor (MBR) process with pre-ozonation compared to an individual MBR using three-dimensional excitation-emission matrix (EEM) fluorescence spectroscopy. While the influent was continuously ozonated at a normal dosage, preferable org. matter removal was achieved in subsequent MBR, and trans-membrane pressure increased at a much lower rate than that of the individual MBR. EEM fluorescence spectroscopy was employed to characterize the dissolved org. matter (DOM) samples, extracellular polymeric substance (EPS) samples and membrane foulants. Four main peaks could be identified from the EEM fluorescence spectra of the DOM samples in both MBRs. Two peaks were assocd. with the protein-like fluorophores, and the other ones were related to the humic-like fluorophores. The results indicated that pre-ozonation decreased fluorescence intensities of all peaks in the EEM spectra of influent DOM esp. for protein-like substances and caused red shifts of all fluorescence peaks to different extents. The peak intensities of the protein-like substances represented by Peak T1 and T2 in EPS spectra were obviously decreased as a result of pre-ozonation. Both external and internal fouling could be effectively mitigated by the pre-ozonation. The most primary component of external foulants was humic acid-like substance (Peak C) in the MBR with pre-ozonation and protein-like substance (Peak T1) in the individual MBR, resp. The content decrease of protein-like substances and structural change of humic-like substances were obsd. in external foulants from EEM fluorescence spectra due to pre-ozonation. However, it could be seen that ozonation resulted in significant redn. of intensities but little location shift of all peaks in EEM fluorescence spectra of internal foulants.
4刘T.;陈志麟;俞，W.-Z.;You， S.-J.使用三维激发发射基质荧光光谱表征浸没式膜生物反应器中的有机膜污染物，并进行预臭氧化。水研究 2011， 45 （5）， 2111– 2121， DOI： 10.1016/j.watres.2010.12.023 - 5Kotlarz, N.; Rockey, N.; Olson, T. M.; Haig, S. J.; Sanford, L.; LiPuma, J. J.; Raskin, L. Biofilms in full-scale drinking water ozone contactors contribute viable bacteria to ozonated water. Environ. Sci. Technol.IF 11.4SCIEJCI 1.44Q1环境科学与生态学1区Top2018, 52 (5), 2618– 2628, DOI: 10.1021/acs.est.7b04212 Google Scholar Google 学术搜索5https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC1cXjtlCktA%253D%253D&md5=b874766ef69b5347cbe6e738dc951156Biofilms in Full-Scale Drinking Water Ozone Contactors Contribute Viable Bacteria to Ozonated WaterKotlarz, Nadine; Rockey, Nicole; Olson, Terese M.; Haig, Sarah-Jane; Sanford, Larry; LiPuma, John J.; Raskin, LutgardeEnvironmental Science & Technology (2018), 52 (5), 2618-2628CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)Concns. of viable microbial cells were monitored using culture-based and culture-independent methods across multichamber ozone contactors in a full-scale drinking water treatment plant. Membrane-intact and culturable cell concns. in ozone contactor effluents ranged from 1200 to 3750 cells/mL and from 200 to 3850 colony forming units/mL, resp. Viable cell concns. decreased significantly in the first ozone contact chamber, but rose, even as ozone exposure increased, in subsequent chambers. Our results implicate microbial detachment from biofilms on contactor surfaces, and from biomass present within lime softening sediments in a hydraulic dead zone, as a possible reason for increasing cell concns. in water samples from sequential ozone chambers. Biofilm community structures on baffle walls upstream and downstream from the dead zone were significantly different from each other (p = 0.017). The biofilms downstream of the dead zone contained a significantly (p = 0.036) higher relative abundance of bacteria of the genera Mycobacterium and Legionella than the upstream biofilms. These results have important implications as the effluent from ozone contactors is often treated further in biol. active filters and bacteria in ozonized water continuously seed filter microbial communities.
5科特拉兹，N.;罗基，N.;奥尔森，TM;黑格，SJ;桑福德，L.;利彪马，J.J.;Raskin， L.全尺寸饮用水臭氧接触器中的生物膜为臭氧水提供了活细菌。环境。科学技术.2018， 52 （5）， 2618– 2628， DOI： 10.1021/acs.est.7b04212 - 6Hammes, F.; Berney, M.; Wang, Y.; Vital, M.; Koster, O.; Egli, T. Flow-cytometric total bacterial cell counts as a descriptive microbiological parameter for drinking water treatment processes. Water Res.IF 12.8SCIEJCI 2.15Q1环境科学与生态学1区Top2008, 42 (1–2), 269– 277, DOI: 10.1016/j.watres.2007.07.009 Google Scholar Google 学术搜索6https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BD2sXhsVGlur%252FF&md5=6ab3931f0b41fa3150749dd4f76f71c9Flow-cytometric total bacterial cell counts as a descriptive microbiological parameter for drinking water treatment processesHammes, Frederik; Berney, Michael; Wang, Yingying; Vital, Marius; Koester, Oliver; Egli, ThomasWater Research (2008), 42 (1-2), 269-277CODEN: WATRAG; ISSN:0043-1354. (Elsevier Ltd.)There are significantly more microbial cells in drinking water than what can be cultured on synthetic growth media. Nonetheless, cultivation-based heterotrophic plate counts (HPCs) are used worldwide as a general microbial quality parameter in drinking water treatment and distribution. Total bacterial cell concns. are normally not considered during drinking water treatment as a design, operative or legislative parameters. This is mainly because easy and rapid methods for quantification of total bacterial cell concns. have, up to now, not been available. As a consequence, the existing lack of data does not allow demonstrating the practical value of this parameter. We used fluorescence staining of microbial cells with the nucleic acid stain SYBR Green I together with quant. flow cytometry (FCM) to analyze total cell concns. in water samples from a drinking water pilot plant. The plant treats surface water (Lake Zuerich) through sequential ozonization, granular activated C (GAC) filtration and membrane ultrafiltration (UF). The data were compared with adenosine tri-phosphate (ATP) measurements and conventional HPCs performed on the same water samples. We demonstrated that the impact of all 3 major treatment steps on the microbiol. in the system could accurately be described with total cell counting: ozonization caused chem. destruction of the bacterial cells; GAC filtration facilitated significant regrowth of the microbial community; and membrane UF phys. removed the bacterial cells from the water. FCM typically detected 1-2 log units more than HPC, while ATP measurements were prone to interference from extracellular ATP released during the ozonation step in the treatment train. We show that total cell concn. measured with FCM is a rapid, easy, sensitive and importantly, a descriptive parameter of several widely applied drinking water treatment processes.
6哈姆斯，F.;伯尼，M.;王彦;维塔尔，M.;科斯特，O.;Egli， T.流式细胞术总细菌细胞计数作为饮用水处理过程的描述性微生物参数。水研究 2008， 42 （1–2）， 269– 277， DOI： 10.1016/j.watres.2007.07.009 - 7Jiang, T.; Tian, T.; Guan, Y.-F.; Yu, H.-Q. Contrasting behaviors of pre-ozonation on ceramic membrane biofouling: Early stage vs late stage. Water Res.IF 12.8SCIEJCI 2.15Q1环境科学与生态学1区Top2022, 220, 118702, DOI: 10.1016/j.watres.2022.118702 Google Scholar Google 学术搜索7https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BB38XhsFGhurnJ&md5=ac3d150b83c4b2f3f122c42c69945e17Contrasting behaviors of pre-ozonation on ceramic membrane biofouling: Early stage vs late stageJiang, Ting; Tian, Tian; Guan, Yan-Fang; Yu, Han-QingWater Research (2022), 220 (), 118702CODEN: WATRAG; ISSN:0043-1354. (Elsevier Ltd.)Pre-ozonation coupled with ceramic membrane filtration has been widely used to alleviate membrane fouling. However, information on the efficiency and underlying mechanism of pre-ozonation in the evolution of ceramic membrane biofouling is limited. Herein, filtration expts. with a synthesis wastewater contg. activated sludge were conducted in a cross-flow system to evaluate the effects of pre-ozonation on ceramic membrane biofouling. Result of flux tests show that pre-ozonation aggravated biofouling at the early stage, but alleviated the biofouling at the late stage. In situ FTIR spectra show that the aggravated biofouling with pre-ozonation was mainly caused by the enhanced complexation between phosphate group from DNA and Al2O3 surface and the increased rigid of proteins' structure. At the early stage, more severe pore blockage further substantiated the higher permeate resistance. By contrast, more dead cells were obsd. on membrane surface at the late stage, indicating the prevention of biofouling development after long-term pre-ozonation. Addnl., the structures and compns. of cake layers at the early and late stages exhibited considerable differences accompanied by the variation in microbial community with the evolution of biofouling. Therefore, this work demonstrates the effectiveness of pre-ozonation in biofouling in long-term operation and provides mechanistic insights into the evolution of biofouling on ceramic membrane.
7蒋婷婷;田，T.;关永芳;Yu， H.-Q.陶瓷膜生物污损预臭氧化的对比行为：早期与晚期。水研究 2022， 220， 118702， DOI： 10.1016/j.watres.2022.118702 - 8Du, J. Y.; Wang, C.; Zhao, Z. W.; Chen, R.; Zhang, P. F.; Cui, F. Y. Effect of vacuum ultraviolet/ozone pretreatment on alleviation of ultrafiltration membrane fouling caused by algal extracellular and intracellular organic matter. ChemosphereIF 8.8SCIEJCI 1.55Q1环境科学与生态学2区Top2022, 305, 135455, DOI: 10.1016/j.chemosphere.2022.135455 Google Scholar Google 学术搜索8https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BB38XhsF2qsrnP&md5=26ba12e172eb505a881aae8f611b9b35Effect of vacuum ultraviolet/ozone pretreatment on alleviation of ultrafiltration membrane fouling caused by algal extracellular and intracellular organic matterDu, Jinying; Wang, Chuang; Zhao, Zhiwei; Chen, Rui; Zhang, Pengfei; Cui, FuyiChemosphere (2022), 305 (), 135455CODEN: CMSHAF; ISSN:0045-6535. (Elsevier Ltd.)Algal blooms in source water can cause algal org. matter (AOM)-related membrane fouling in drinking water treatment. Herein, the effects of vacuum UV/ozone (VUV/O3) pretreatment on alleviating ultrafiltration membrane fouling caused by AOM, including extracellular org. matter (EOM) and intracellular org. matter (IOM), were investigated systematically. Compared to its sub-processes (UV/O3, O3, VUV, and UV), VUV/O3 pretreatment showed the best performance on AOM removal and membrane fouling mitigation. After VUV/O3 pretreatment, the DOC of EOM and IOM in feed decreased by 51.1% and 26.7%, resp., and fluorescence components and UV254 of EOM and IOM in feed decreased obviously. Hence, the final specific fluxes of the membranes increased significantly under the impacts of VUV/O3, and VUV/O3 achieved 89.5% and 97.2% mitigation of reversible fouling caused by EOM and IOM, resp. VUV/O3 pretreatment also reduced the foulants on membrane surface and surface roughness. Moreover, under the effects of reactive oxygen species oxidn., VUV photolysis, and direct O3 oxidn., VUV/O3 decreased org. load and changed the mol. wt. distribution, hydrophilicity, and interaction-free energy of AOM, thus mitigating membrane fouling. Furthermore, the effects of O3 dosage and mol. wt. cut-off of ultrafiltration membrane on membrane fouling mitigation by VUV/O3 were also investigated. All results highlighted that VUV/O3 pretreatment had huge potential in mitigating AOM-induced membrane fouling.
8杜，J.Y.;王，C.;赵志伟;陈，R.;张，P.F.;真空紫外/臭氧预处理对缓解藻类细胞外和细胞内有机物引起的超滤膜污染的影响.化学圈2022， 305， 135455， DOI： 10.1016/j.chemosphere.2022.135455 - 9Yu, W.; Liu, T.; Crawshaw, J.; Liu, T.; Graham, N. Ultrafiltration and nanofiltration membrane fouling by natural organic matter: Mechanisms and mitigation by pre-ozonation and pH. Water Res.IF 12.8SCIEJCI 2.15Q1环境科学与生态学1区Top2018, 139, 353– 362, DOI: 10.1016/j.watres.2018.04.025 Google Scholar Google 学术搜索9https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC1cXns1WmsLs%253D&md5=420aabcd3a3d86d667c671cfbf6ea2f5Ultrafiltration and nanofiltration membrane fouling by natural organic matter: Mechanisms and mitigation by pre-ozonation and pHYu, Wenzheng; Liu, Teng; Crawshaw, John; Liu, Ting; Graham, NigelWater Research (2018), 139 (), 353-362CODEN: WATRAG; ISSN:0043-1354. (Elsevier Ltd.)The fouling of ultrafiltration (UF) and nanofiltration (NF) membranes during the treatment of surface waters continues to be of concern and the particular role of natural org. matter (NOM) requires further investigation. In this study the effect of pH and surface charge on membrane fouling during the treatment of samples of a representative surface water (Hyde Park recreational lake) were evaluated, together with the impact of pre-ozonation. While biopolymers in the surface water could be removed by the UF membrane, smaller mol. wt. (MW) fractions of NOM were poorly removed, confirming the importance of membrane pore size. For NF membranes the removal of smaller MW fractions (800Da-10kDa) was less than expected from their pore size; however, nearly all of the hydrophobic, humic-type substances could be removed by the hydrophilic NF membranes for all MW distributions (greater than 90%). The results indicated the importance of the charge and hydrophilic nature of the NOM. Thus, the hydrophilic NF membrane could remove the hydrophobic org. matter, but not the hydrophilic substances. Increasing charge effects (more neg. zeta potentials) with increasing soln. pH were found to enhance orgs. removal and reduce fouling (flux decline), most likely through greater membrane surface repulsion. Pre-ozonation of the surface water increased the hydrophilic fraction and anionic charge of NOM and altered their size distributions. This resulted in a decreased fouling (less flux decline) for the UF and smaller pore NF, but a slight increase in fouling for the larger pore NF. The differences in the NF behavior are believed to relate to the relative sizes of ozonated org. fractions and the NF pores; a similar size of ozonated org. fractions and the NF pores causes significant membrane fouling.
9余，W.;刘婷婷;克劳肖，J.;刘婷婷;Graham， N.天然有机物的超滤和纳滤膜污染：预臭氧和pH值的机制和缓解。水研究 2018， 139， 353– 362， DOI： 10.1016/j.watres.2018.04.025 - 10Wang, L.; Song, S.; Xu, L.; Graham, N. J. D.; Yu, W. Z. Beneficial role of pre- and post-ozonation in a low rate biofiltration-ultrafiltration process treating reclaimed water. Water Res.IF 12.8SCIEJCI 2.15Q1环境科学与生态学1区Top2022, 226, 119284, DOI: 10.1016/j.watres.2022.119284 Google Scholar Google 学术搜索There is no corresponding record for this reference.
10王玲玲;宋，S.;徐，L.;格雷厄姆，新泽西州;Yu， W. Z.臭氧化前和臭氧后在处理再生水的低速率生物过滤-超滤过程中的有益作用。水研究 2022， 226， 119284， DOI： 10.1016/j.watres.2022.119284 - 11Jennings, E.; Kremser, A.; Han, L. M.; Reemtsma, T.; Lechtenfeld, O. J. Discovery of polar ozonation byproducts via direct injection of effluent organic matter with online LC-FT-ICR-MS. Environ. Sci. Technol.IF 11.4SCIEJCI 1.44Q1环境科学与生态学1区Top2022, 56 (3), 1894– 1904, DOI: 10.1021/acs.est.1c04310 Google Scholar Google 学术搜索11https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BB38XlvVCjtg%253D%253D&md5=612f9cbdc1d13d9f3af1c3c92ebc33c8Discovery of polar ozonation byproducts via direct injection of effluent organic matter with online LC-FT-ICR-MSJennings, Elaine; Kremser, Arina; Han, Limei; Reemtsma, Thorsten; Lechtenfeld, Oliver J.Environmental Science & Technology (2022), 56 (3), 1894-1904CODEN: ESTHAG; ISSN:1520-5851. (American Chemical Society)Effluent org. matter (EfOM), a major ozone consumer during wastewater ozonation, is a complex mixt. of natural and anthropogenic org. mols. Ozonation of EfOM adds to mol. complexity by introducing polar and potentially mobile ozonation byproducts (OBPs). Currently, nontargeted direct infusion (DI) ultrahigh resoln. mass spectrometry (e.g. FT-ICR-MS) is used to study OBPs but requires sample extn., limiting the accessible polarity range of OBPs. To better understand the impact of ozonation on EfOM and the formation of polar OBPs, nonextd. effluent was analyzed by direct injection onto a reversed-phase liq. chromatog. system (RP-LC) online hyphenated with an FT-ICR-MS. Over four times more OBPs were detected in nonextd. EfOM compared to effluent extd. with solid phase extn. and measured with DI-FT-ICR-MS (13817 vs 3075). Over 1500 highly oxygenated OBPs were detected exclusively in early eluting fractions of nonextd. EfOM, indicating polar OBPs. Oxygenation of these newly discovered OBPs is higher than previously found, with an av. mol. DBE-O value of -3.3 and O/C ratio of 0.84 in the earliest eluting OBP fractions. These polar OBPs are consistently lost during extn. but may play an important role in understanding the environmental impact of ozonated EfOM. Moreover, 316 mol. formulas classified as nonreactive to ozone in DI-FT-ICR-MS can be identified with LC-FT-ICR-MS as isomers with varying degrees of reactivity, providing for the first time exptl. evidence of differential reactivity of complex org. matter isomers with ozone.
11詹宁斯，E.;克雷姆瑟，A.;韩，L.M.;雷姆茨玛，T.;Lechtenfeld， O. J.通过在线LC-FT-ICR-MS直接注入废水有机物发现极性臭氧化副产物。环境。科学技术.2022， 56 （3）， 1894– 1904， DOI： 10.1021/acs.est.1c04310 - 12Phungsai, P.; Kurisu, F.; Kasuga, I.; Furumai, H. Changes in dissolved organic matter composition and disinfection byproduct precursors in advanced drinking water treatment processes. Environ. Sci. Technol.IF 11.4SCIEJCI 1.44Q1环境科学与生态学1区Top2018, 52 (6), 3392– 3401, DOI: 10.1021/acs.est.7b04765 Google Scholar Google 学术搜索12https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC1cXjtVemurk%253D&md5=7f763252275b4c420cda1a79feab6d19Changes in Dissolved Organic Matter Composition and Disinfection Byproduct Precursors in Advanced Drinking Water Treatment ProcessesPhungsai, Phanwatt; Kurisu, Futoshi; Kasuga, Ikuro; Furumai, HiroakiEnvironmental Science & Technology (2018), 52 (6), 3392-3401CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)Mol. changes in dissolved org. matter (DOM) from treatment processes at two drinking water treatment plants in Japan were investigated using unknown screening anal. by Orbitrap mass spectrometry. DOM formulas with carbon, hydrogen and oxygen (CHO-DOM) were the most abundant class in water samples, and over half of them were commonly found at both plants. Among the treatment processes, ozonization induced the most drastic changes to DOM. Mass peak intensities of less satd. CHO-DOM (pos. (oxygen subtracted double bond equiv. per carbon (DBE-O)/C)) decreased by ozonization, while more satd. oxidn. byproducts (neg. (DBE-O)/C) increased and new oxidn. byproducts (OBPs) were detected. By Kendrick mass anal., ozone reactions preferred less satd. CHO-DOM in the same alkylation families and produced more satd. alkylation families of OBPs. Following ozonization, biol. activated carbon filtration effectively removed <300 Da CHO-DOM, including OBPs. Following chlorination, over 50 chlorinated formulas of disinfection byproducts (DBPs) were found in chlorinated water samples where at least half were unknown. Putative precursors of these DBPs were detd. based on electrophilic substitutions and addn. reactions. Ozonization demonstrated better decompn. of addn. reaction-type precursors than electrophilic substitution-type precursors; over half of both precursor types decreased during biol. activated carbon filtration.
12Phungsai，P.;栗树，F.;春日，I.;Furumai， H.先进饮用水处理工艺中溶解有机物组成和消毒副产物前体的变化。环境。科学技术.2018， 52 （6）， 3392– 3401， DOI： 10.1021/acs.est.7b04765 - 13von Gunten, U. Ozonation of drinking water: Part I. Oxidation kinetics and product formation. Water Res.IF 12.8SCIEJCI 2.15Q1环境科学与生态学1区Top2003, 37 (7), 1443– 1467, DOI: 10.1016/S0043-1354(02)00457-8 Google Scholar Google 学术搜索13https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BD3sXhtlGqsr4%253D&md5=a71315929c55e466b0f0f0a8908eebb3Ozonation of drinking water: Part I. Oxidation kinetics and product formationvon Gunten, UrsWater Research (2003), 37 (7), 1443-1467CODEN: WATRAG; ISSN:0043-1354. (Elsevier Science Ltd.)A review is given. The oxidn. of org. and inorg. compds. during ozonization can occur via ozone or OH radicals or a combination thereof. The oxidn. pathway is detd. by the ratio of ozone and OH radical concns. and the corresponding kinetics. A huge database with several hundred rate consts. for ozone and a few thousand rate consts. for OH radicals is available. Ozone is an electrophile with a high selectivity. The 2nd-order rate consts. for oxidn. by ozone vary over 10 orders of magnitude, <0.1-7 × 109/M-s. The reactions of ozone with drinking-water relevant inorg. compds. are typically fast and occur by an oxygen atom transfer reaction. Org. micropollutants are oxidized with ozone selectively. Ozone reacts mainly with double bonds, activated arom. systems and non-protonated amines. In general, electron-donating groups enhance the oxidn. by ozone whereas electron-withdrawing groups reduce the reaction rates. The kinetics of direct ozone reactions depend strongly on the speciation (acid-base, metal complexation). The reaction of OH radicals with the majority of inorg. and org. compds. is nearly diffusion-controlled. The degree of oxidn. by ozone and OH radicals is given by the corresponding kinetics. Product formation from the ozonation of org. micropollutants in aq. systems has only been established for a few compds.
13von Gunten，U.饮用水的臭氧作用：第一部分，氧化动力学和产物形成。水研究 2003， 37 （7）， 1443– 1467， DOI： 10.1016/S0043-1354（02）00457-8 - 14von Gunten, U. Ozonation of drinking water: Part II. Disinfection and by-product formation in presence of bromide, iodide or chlorine. Water Res.IF 12.8SCIEJCI 2.15Q1环境科学与生态学1区Top2003, 37 (7), 1469– 1487, DOI: 10.1016/S0043-1354(02)00458-X Google Scholar Google 学术搜索14https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BD3sXhtlGqsr8%253D&md5=ba68eddfcd8c59a62e16885393b6f0d5Ozonation of drinking water: Part II. Disinfection and by-product formation in presence of bromide, iodide or chlorinevon Gunten, UrsWater Research (2003), 37 (7), 1469-1487CODEN: WATRAG; ISSN:0043-1354. (Elsevier Science Ltd.)A review is given. Proper rate consts. for the inactivation of microorganisms are only available for 6 species (E. coli, Bacillus subtilis spores, Rotavirus, Giardia lamblia cysts, Giardia muris cysts, Cryptosporidium parvum oocysts). The apparent activation energy for the inactivation of bacteria is in the same order as most chem. reactions (35-50 KJ/mol), whereas it is much higher for the inactivation of protozoa (80 KJ/mol). This requires significantly higher ozone exposures at low temps. to get a similar inactivation for protozoa. Even for the inactivation of resistant microorganisms, OH radicals only play a minor role. Numerous org. and inorg. ozonation disinfection/oxidn. byproducts have been identified. The byproduct of main concern is bromate, which is formed in bromide-contg. waters. A low drinking water std. of 10 μg/L has been set for bromate. Therefore, disinfection and oxidn. processes have to be evaluated to fulfil these criteria. In certain cases, when bromide concns. are above about 50 μg/L, it may be necessary to use control measures to lower bromate formation (lowering of pH, ammonia addn.). Iodate is the main byproduct formed during ozonation of iodide-contg. waters. The reactions involved are direct ozone oxidns. Iodate is considered non-problematic because it is transformed back to iodide endogenically. Chloride cannot be oxidized during ozonation processes under drinking water conditions. Chlorate is only formed if a preoxidn. by chlorine and/or chlorine dioxide has occurred.
14von Gunten，U.饮用水臭氧化：第二部分。在溴化物、碘化物或氯存在下进行消毒和副产物形成。水研究 2003， 37 （7）， 1469– 1487， DOI： 10.1016/S0043-1354（02）00458-X - 15Wenk, J.; Aeschbacher, M.; Salhi, E.; Canonica, S.; von Gunten, U.; Sander, M. Chemical oxidation of dissolved organic matter by chlorine dioxide, chlorine, and ozone: Effects on its optical and antioxidant properties. Environ. Sci. Technol.IF 11.4SCIEJCI 1.44Q1环境科学与生态学1区Top2013, 47 (19), 11147– 11156, DOI: 10.1021/es402516b Google Scholar Google 学术搜索15https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC3sXhtleksbbE&md5=11bda373fa816d65351e83e1b8e3b9f1Chemical Oxidation of Dissolved Organic Matter by Chlorine Dioxide, Chlorine, and Ozone: Effects on Its Optical and Antioxidant PropertiesWenk, Jannis; Aeschbacher, Michael; Salhi, Elisabeth; Canonica, Silvio; von Gunten, Urs; Sander, MichaelEnvironmental Science & Technology (2013), 47 (19), 11147-11156CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)In water treatment dissolved org. matter (DOM) is typically the major sink for chem. oxidants. The resulting changes in DOM, such as its optical properties have been measured to follow the oxidn. processes. However, such measurements contain only limited information on the changes in the oxidn. states of and the reactive moieties in the DOM. We used mediated electrochem. oxidn. to quantify changes in the electron donating capacities (EDCs), and hence the redox states, of 3 different types of DOM during oxidn. with ClO2, Cl (as HOCl/OCl-), and O3. Treatment with ClO2 and HOCl resulted in comparable and prominent decreases in EDCs, while the UV light absorbances of the DOM decreased only slightly. Conversely, ozonization resulted in only small decreases of the EDCs but pronounced absorbance losses of the DOM. These results suggest that ClO2 and HOCl primarily reacted as oxidants by accepting electrons from electron-rich phenolic and hydroquinone moieties in the DOM, while O3 reacted via electrophilic addn. to arom. moieties, followed by ring cleavage. This study highlights the potential of combined EDC-UV measurements to monitor chem. oxidn. of DOM, to assess the nature of the reactive moieties and to study the underlying reaction pathways.
15温克，J.;埃施巴赫，M.;萨利希，E.;卡诺尼卡，S.;von Gunten，美国;Sander， M.二氧化氯、氯和臭氧对溶解有机物的化学氧化：对其光学和抗氧化性能的影响。环境。Sci. Technol.2013， 47 （19）， 11147– 11156， DOI： 10.1021/es402516b - 16Remucal, C. K.; Salhi, E.; Walpen, N.; von Gunten, U. Molecular-level transformation of dissolved organic matter during oxidation by ozone and hydroxyl radical. Environ. Sci. Technol.IF 11.4SCIEJCI 1.44Q1环境科学与生态学1区Top2020, 54 (16), 10351– 10360, DOI: 10.1021/acs.est.0c03052 Google Scholar Google 学术搜索16https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BB3cXhsVegt7zE&md5=f98f8139a31c6facb1fd377748fb2c28Molecular-level transformation of dissolved organic matter during oxidation by ozone and hydroxyl radicalRemucal, Christina K.; Salhi, Elisabeth; Walpen, Nicolas; von Gunten, UrsEnvironmental Science & Technology (2020), 54 (16), 10351-10360CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)Ozonation of drinking and wastewater relies on ozone (O3) and hydroxyl radical (•OH) as oxidants. Both oxidants react with dissolved org. matter (DOM) and alter its compn., but the selectivity of the two oxidants and mechanisms of reactivity with DOM moieties are largely unknown. The reactions of O3 and •OH with two DOM isolates were studied by varying specific ozone doses (0.1-1.3 mg-O3/mg-C) at pH 7. Addnl., conditions that favor O3 (i.e., addn. of an •OH scavenger) or •OH (i.e., pH 11) were investigated. Ozonation decreases aromaticity, apparent mol. wt., and electron donating capacity (EDC) of DOM with large changes obsd. when O3 is the main oxidant (e.g., EDC decreases 63-77% for 1.3 mg-O3/mg-C). Both O3 and •OH react with highly arom., reduced formulas detected using high-resoln. mass spectrometry (O:C = 0.48 ± 0.12; H:C = 1.06 ± 0.23), while •OH also oxidizes more satd. formulas (H:C = 1.64 ± 0.26). Established reactions between model compds. and O3 (e.g., addn. of one to two oxygen atoms) or •OH (e.g., addn. of one oxygen atom and decarboxylation) are obsd. and produce highly oxidized DOM (O:C > 1.0). This study provides mol.-level evidence for the selectivity of O3 as an oxidant within DOM.
16雷穆卡尔，C.K.;萨利希，E.;沃尔彭，N.;von Gunten，U.臭氧和羟基自由基氧化过程中溶解有机物的分子水平转化。环境。科学技术.2020， 54 （16）， 10351– 10360， DOI： 10.1021/acs.est.0c03052 - 17Camel, V.; Bermond, A. The use of ozone and associated oxidation processes in drinking water treatment. Water Res.IF 12.8SCIEJCI 2.15Q1环境科学与生态学1区Top1998, 32 (11), 3208– 3222, DOI: 10.1016/S0043-1354(98)00130-4 Google Scholar Google 学术搜索17https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADyaK1cXmslaqtrs%253D&md5=cd3b8501013d0719470cdc43fa41fb5fThe use of ozone and associated oxidation processes in drinking water treatmentCamel, V.; Bermond, A.Water Research (1998), 32 (11), 3208-3222CODEN: WATRAG; ISSN:0043-1354. (Elsevier Science Ltd.)A review, with many refs., summarizes the main applications of ozonization and assocd. oxidn. processes in the treatment of surface water and groundwater for drinking water prodn. Oxidants may be added at several points throughout the treatment: pre-oxidn., intermediate oxidn. or final disinfection. So, the numerous effects of chem. oxidn. are discussed along the water treatment: removal of inorg. species, aid to the coagulation-flocculation process, degrdn. of org. matter and disinfection. Of prime importance in potable water prodn. is the removal of org. matter (natural humic substances, as well as micropollutants, esp. pesticides) to avoid degrdn. of the distributed water (mainly bad odors and tastes; formation of disinfection byproducts such as trihalomethanes; microbial regrowth in the distribution system). Consequently, this point has been particularly detailed. Complete mineralization hardly occurs during the process; as a consequence, further treatment (i.e. sand or granular activated C filtration) is required to improve the distributed water quality, and to meet the drinking water regulations.
17骆驼，V.;Bermond， A.臭氧和相关氧化过程在饮用水处理中的应用。水研究 1998， 32 （11）， 3208– 3222， DOI： 10.1016/S0043-1354（98）00130-4 - 18Headley, J. V.; Kumar, P.; Dalai, A.; Peru, K. M.; Bailey, J.; McMartin, D. W.; Rowland, S. M.; Rodgers, R. P.; Marshall, A. G. Fourier transform ion cyclotron resonance mass spectrometry characterization of treated Athabasca oil sands processed waters. Energy FuelsIF 5.3SCIEJCI 0.66Q1工程技术3区2015, 29 (5), 2768– 2773, DOI: 10.1021/ef502007b Google Scholar Google 学术搜索18https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC2cXhvVygsrjP&md5=a886900067d550434bde1829101028b1Fourier Transform Ion Cyclotron Resonance Mass Spectrometry Characterization of Treated Athabasca Oil Sands Processed WatersHeadley, John V.; Kumar, Pardeep; Dalai, Ajay; Peru, Kerry M.; Bailey, Jon; McMartin, Dena W.; Rowland, Steven M.; Rodgers, Ryan P.; Marshall, Alan G.Energy & Fuels (2015), 29 (5), 2768-2773CODEN: ENFUEM; ISSN:0887-0624. (American Chemical Society)Ultrahigh-resoln. neg.-ion electrospray ionization Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS) was used to characterize Athabasca oil sands processed water (OSPW) treated by (A) coagulation flocculent with lime and bentonite, (B) coagulation flocculent with lime and bentonite followed by activated carbon, and (C) combined ozonation and ultrasonication. Treatment A was ineffective in reducing the level of total naphthenic acid fraction components [NAFCs, defined as the acid-extractable fraction of OSPWs or crude oils (CnH2n + zOwSxNy), where the values n, w, x, and y indicate the no. of carbon, oxygen, sulfur, and nitrogen atoms, resp., and z represents the hydrogen atom deficiency because of the presence of double bonds and ring formation]. Likewise, for treatment A, little or no change was obsd. for the double bond equiv. (DBE) distributions of the compd. classes. Treatments B and C resulted in the redn. of total NAFCs by 26 ± 1.4 and 89 ± 1.1%, resp. For the latter treatments, there was evidence for selective removal of the S and OxSy heteroat. species at the mol. level, along with a redn. in the DBE values for all species.
18海德利，J.V.;库马尔，P.;达赖，A.;秘鲁，K.M.;贝利，J.;麦克马丁，DW;罗兰，SM;罗杰斯，RP;Marshall， A. G.傅里叶变换离子回旋共振质谱表征处理过的阿萨巴斯卡油砂加工水。能源燃料2015， 29 （5）， 2768– 2773， DOI： 10.1021/ef502007b - 19Scholes, R. C.; King, J. F.; Mitch, W. A.; Sedlak, D. L. Transformation of trace organic contaminants from reverse osmosis concentrate by open-water unit-process wetlands with and without ozone pretreatment. Environ. Sci. Technol.IF 11.4SCIEJCI 1.44Q1环境科学与生态学1区Top2020, 54 (24), 16176– 16185, DOI: 10.1021/acs.est.0c04406 Google Scholar Google 学术搜索19https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BB3cXisVGhu7bF&md5=306159352fefb5abcfcb2b1a97410294Transformation of trace organic contaminants from reverse osmosis concentrate by open-water unit-process wetlands with and without ozone pretreatmentScholes, Rachel C.; King, Jacob F.; Mitch, William A.; Sedlak, David L.Environmental Science & Technology (2020), 54 (24), 16176-16185CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)Reverse osmosis (RO) treatment of municipal wastewater effluent is becoming more common as water reuse is implemented in water-stressed regions. Where RO conc. is discharged with limited diln., concns. of trace org. contaminants could pose risks to aquatic ecosystems. To provide a low-cost option for removing trace org. compds. from RO conc., a pilot-scale treatment system comprising open-water unit-process wetlands with and without ozone pretreatment was studied over a 2-yr period. A suite of ecotoxicol. relevant org. contaminants was partially removed via photo- and bio-transformations, including β-adrenergic blockers, antivirals, antibiotics, and pesticides. Biotransformation rates were as fast as or up to approx. 50% faster than model predictions based upon data from open-water wetlands that treated municipal wastewater effluent. Phototransformation rates were comparable to or as much as 60% slower than those predicted by models that accounted for light penetration and scavenging of reactive oxygen species. Several compds. were transformed during ozone pretreatment that were poorly removed in the open-water wetland. The combined treatment system resulted in a decrease in the risk quotients of trace org. contaminants in the RO conc., but still diln. may be required to protect sensitive species from urban-use pesticides with low environmental effect concns.
19斯科尔斯，R.C.;金，J.F.;米奇，WA;Sedlak， D. L.通过开放水域单元工艺湿地在有和没有臭氧预处理的情况下转化反渗透浓缩物中的痕量有机污染物。环境。科学技术.2020， 54 （24）， 16176– 16185， DOI： 10.1021/acs.est.0c04406 - 20Hubner, U.; von Gunten, U.; Jekel, M. Evaluation of the persistence of transformation products from ozonation of trace organic compounds: A critical review. Water Res.IF 12.8SCIEJCI 2.15Q1环境科学与生态学1区Top2015, 68, 150– 170, DOI: 10.1016/j.watres.2014.09.051 Google Scholar Google 学术搜索There is no corresponding record for this reference.
20Hubner，美国;von Gunten，美国;Jekel， M.微量有机化合物臭氧转化产物的持久性评估：批判性综述。水研究 2015， 68， 150– 170， DOI： 10.1016/j.watres.2014.09.051 - 21Papageorgiou, A.; Voutsa, D.; Papadakis, N. Occurrence and fate of ozonation by-products at a full-scale drinking water treatment plant. Sci. Total Environ.IF 9.8SCIEJCI 1.68Q1环境科学与生态学1区Top2014, 481, 392– 400, DOI: 10.1016/j.scitotenv.2014.02.069 Google Scholar Google 学术搜索21https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC2cXmtVWlu70%253D&md5=cc25f743eb20af754605612b81b94ea0Occurrence and fate of ozonation by-products at a full-scale drinking water treatment plantPapageorgiou, A.; Voutsa, D.; Papadakis, N.Science of the Total Environment (2014), 481 (), 392-400CODEN: STENDL; ISSN:0048-9697. (Elsevier B.V.)Occurrence and fate of carbonyl compds. as ozonation byproducts at a full scale drinking water treatment plant (DWTP) were studied for 1 yr. Raw water and post-treatment samples (pre-ozonation, coagulation/flocculation, sand filtration, main ozonation, granular activated C filtration, chlorination) were collected monthly. Pre-ozonation formed carbonyl compds. at 67.3 ± 43.3 μg/L as the sum of 14 carbonyl compds.; lower concns. were detd. following the main ozonation process, 32.8 ± 22.3 μg/L. Dominant compds. were formaldehyde, acetaldehyde, glyoxal, and Me glyoxal, contributing 65% of total carbonyl content. Dissolved org. C reactivity for carbonyl compd. formation varied throughout the year, exhibiting higher values in spring. Coagulation/flocculation and sand filtration significantly removed (64-80%) carbonyl compds. formed in the pre-ozonation step. Granular activated C filtration removal efficiency exhibited great variation, 15-62%. Carbonyl compd. concns. in finished water were low, close to detection limits, showed the efficiency of DWTP in removing this class of ozonation byproducts.
21帕帕乔吉乌，A.;武察，D.;Papadakis，N.全尺寸饮用水处理厂臭氧化副产物的发生和归宿。Sci. Total Environ.2014， 481， 392– 400， DOI： 10.1016/j.scitotenv.2014.02.069 - 22Sun, W.; Lu, Z.; Zhang, Z.; Zhang, Y.; Shi, B.; Wang, H. Ozone and fenton oxidation affected the bacterial community and opportunistic pathogens in biofilms and effluents from GAC. Water Res.IF 12.8SCIEJCI 2.15Q1环境科学与生态学1区Top2022, 218, 118495, DOI: 10.1016/j.watres.2022.118495 Google Scholar Google 学术搜索There is no corresponding record for this reference.
22日，W.;卢，Z.;张志强;张勇;石，B.;Wang、H.Ozone和Fenton氧化影响了GAC生物膜和废水中的细菌群落和机会性病原体。水研究 2022， 218， 118495， DOI： 10.1016/j.watres.2022.118495 - 23Ratzke, C.; Barrere, J.; Gore, J. Strength of species interactions determines biodiversity and stability in microbial communities. Nat. Ecol. Evol.IF 16.8SCIEJCI 3.93Q1生物学1区Top2020, 4, 376– 383, DOI: 10.1038/s41559-020-1099-4 Google Scholar Google 学术搜索23https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A280%3ADC%252BB387gsFWqtA%253D%253D&md5=1300026b85935909ddb38ad2b9172093Strength of species interactions determines biodiversity and stability in microbial communitiesRatzke Christoph; Barrere Julien; Gore Jeff; Barrere JulienNature ecology & evolution (2020), 4 (3), 376-383 ISSN:.Organisms-especially microbes-tend to live together in ecosystems. While some of these ecosystems are very biodiverse, others are not, and while some are very stable over time, others undergo strong temporal fluctuations. Despite a long history of research and a plethora of data, it is not fully understood what determines the biodiversity and stability of ecosystems. Theory and experiments suggest a connection between species interaction, biodiversity and the stability of ecosystems, where an increase in ecosystem stability with biodiversity could be observed in several cases. However, what causes these connections remains unclear. Here, we show in microbial ecosystems in the laboratory that the concentrations of available nutrients can set the strength of interactions between bacteria. High nutrient concentrations allowed the bacteria to strongly alter the chemical environment, causing on average more negative interactions between species. These stronger interactions excluded more species from the community, resulting in a loss of biodiversity. At the same time, the stronger interactions also decreased the stability of the microbial communities, providing a mechanistic link between species interaction, biodiversity and stability in microbial ecosystems.
23拉茨克，C.;巴雷尔，J.;Gore， J.物种相互作用的强度决定了微生物群落的生物多样性和稳定性。Nat. Ecol. Evol.2020， 4， 376– 383， DOI： 10.1038/s41559-020-1099-4 - 24Desmond, P.; Best, J. P.; Morgenroth, E.; Derlon, N. Linking composition of extracellular polymeric substances (EPS) to the physical structure and hydraulic resistance of membrane biofilms. Water Res.IF 12.8SCIEJCI 2.15Q1环境科学与生态学1区Top2018, 132, 211– 221, DOI: 10.1016/j.watres.2017.12.058 Google Scholar Google 学术搜索24https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC1cXntlGntg%253D%253D&md5=8ad69e3d237d15096e8844ad9229fcc5Linking composition of extracellular polymeric substances (EPS) to the physical structure and hydraulic resistance of membrane biofilmsDesmond, Peter; Best, James P.; Morgenroth, Eberhard; Derlon, NicolasWater Research (2018), 132 (), 211-221CODEN: WATRAG; ISSN:0043-1354. (Elsevier Ltd.)The effect of extracellular polymeric substances (EPS) on the meso-scale phys. structure and hydraulic resistance of membrane biofilms during gravity driven membrane (GDM) filtration was investigated. Biofilms were developed on the surface of ultrafiltration membranes during dead-end filtration at ultra-low pressure (70mbar). Biofilm EPS compn. (total protein, polysaccharide and eDNA) was manipulated by growing biofilms under contrasting nutrient conditions. Nutrient conditions consisted of (i) a nutrient enriched condition with a nutrient ratio of 100:30:10 (C: N: P), (ii) a phosphorus limitation (C: N: P ratio: 100:30:0), and (iii) a nitrogen limitation (C: N: P ratio: 100:0:10). The structure of the biofilm was characterised at meso-scale using Optical Coherence Tomog. (OCT). Biofilm compn. was analyzed with respect to total org. carbon, total cellular mass and extracellular concns. of proteins, polysaccharides, and eDNA. 2D-confocal Raman mapping was used to characterize the functional group compn. and micro-scale distribution of the biofilms EPS. Our study reveals that the compn. of the EPS matrix can det. the meso-scale phys. structure of membrane biofilms and in turn its hydraulic resistance. Biofilms grown under P limiting conditions were characterised by dense and homogeneous phys. structures with high concns. of polysaccharides and eDNA. Biofilm grown under nutrient enriched or N limiting conditions were characterised by heterogeneous phys. structures with lower concns. of polysaccharides and eDNA. For P limiting biofilms, 2D-confocal Raman microscopy revealed a homogeneous spatial distribution of anionic functional groups in homogeneous biofilm structures with higher polysaccharide and eDNA concns. This study links EPS compn., phys. structure and hydraulic resistance of membrane biofilms, with practical relevance for the hydraulic performances of GDM ultrafiltration.
24德斯蒙德，P.;最佳，J.P.;摩根罗斯，E.;Derlon， N.将细胞外聚合物物质（EPS）的组成与膜生物膜的物理结构和水力阻力联系起来。水研究 2018， 132， 211– 221， DOI： 10.1016/j.watres.2017.12.058 - 25Desmond, P.; Morgenroth, E.; Derlon, N. Physical structure determines compression of membrane biofilms during gravity driven membrane (GDM) ultrafiltration. Water Res.IF 12.8SCIEJCI 2.15Q1环境科学与生态学1区Top2018, 143, 539– 549, DOI: 10.1016/j.watres.2018.07.008 Google Scholar Google 学术搜索There is no corresponding record for this reference.
25德斯蒙德，P.;摩根罗斯，E.;Derlon， N.物理结构决定了重力驱动膜 （GDM） 超滤过程中膜生物膜的压缩。水研究 2018， 143， 539– 549， DOI： 10.1016/j.watres.2018.07.008 - 26Zhang, L.; Graham, N.; Derlon, N.; Tang, Y.; Siddique, M. S.; Xu, L.; Yu, W. Biofouling by ultra-low pressure filtration of surface water: The paramount role of initial available biopolymers. J. Membr. Sci.IF 9.5SCIEJCI 1.85Q1工程技术1区Top2021, 640, 119740, DOI: 10.1016/j.memsci.2021.119740 Google Scholar Google 学术搜索26https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BB3MXhvFCrt77O&md5=3e8eab80565dce0b9576d35cd0537559Biofouling by ultra-low pressure filtration of surface water: The paramount role of initial available biopolymersZhang, Li; Graham, Nigel; Derlon, Nicolas; Tang, Youneng; Siddique, Muhammad Saboor; Xu, Lei; Yu, WenzhengJournal of Membrane Science (2021), 640 (), 119740CODEN: JMESDO; ISSN:0376-7388. (Elsevier B.V.)Biofouling layer (i.e., biofilm) is an inevitable presence for the membrane filtration processes. In this study, we elucidated biofouling formation from the perspective of affecting the attachment of bacteria for the first time, whereby the role of initial available biopolymers was revealed. Results demonstrated that the presence of initial available biopolymers increased the abundance of the genus Caulobacter, which was capable of mineralizing biopolymers; whereas, for the typically oligotrophic species of Polynucleobacter, it exhibited low abundance. Greater concns. of polysaccharides and proteins were accumulated in the biofouling layer, when provided with initial biopolymers, and the biofilm structure was more heterogeneous with larger pore size and higher thickness. Thereby, the corresponding filtration system exhibited greater permeability and better removal performance of orgs. Collectively, the initial available biopolymers altered the attachment conditions for the bacteria, which subsequently impacted the bacterial community, and in turn biofilm compn., phys. structure and filtration performance.
26张，L.;格雷厄姆，N.;德隆，N.;唐彦;西迪克，MS;徐，L.;Yu， W.通过地表水的超低压过滤进行生物污染：初始可用生物聚合物的首要作用。J.门布尔。Sci.2021， 640， 119740， DOI： 10.1016/j.memsci.2021.119740 - 27Tanentzap, A. J.; Fitch, A.; Orland, C.; Emilson, E. J. S.; Yakimovich, K. M.; Osterholz, H.; Dittmar, T. Chemical and microbial diversity covary in fresh water to influence ecosystem functioning. Proc. Natl. Acad. Sci. U.S.A.IF 11.1SCIEJCI 2.52Q1综合性期刊1区Top2019, 116 (49), 24689– 24695, DOI: 10.1073/pnas.1904896116 Google Scholar Google 学术搜索27https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC1MXitlejsLrM&md5=32a8b202a055c153ca8e479212707fd9Chemical and microbial diversity covary in fresh water to influence ecosystem functioningTanentzap, Andrew J.; Fitch, Amelia; Orland, Chloe; Emilson, Erik J. S.; Yakimovich, Kurt M.; Osterholz, Helena; Dittmar, ThorstenProceedings of the National Academy of Sciences of the United States of America (2019), 116 (49), 24689-24695CODEN: PNASA6; ISSN:0027-8424. (National Academy of Sciences)Invisible to the naked eye lies a tremendous diversity of org. mols. and organisms that make major contributions to important biogeochem. cycles. However, how the diversity and compn. of these two communities are interlinked remains poorly characterized in fresh waters, despite the potential for chem. and microbial diversity to promote one another. Here we exploited gradients in chemodiversity within a common microbial pool to test how chem. and biol. diversity covary and characterized the implications for ecosystem functioning. We found that both chemodiversity and genes assocd. with org. matter decompn. increased as more plant litterfall accumulated in exptl. lake sediments, consistent with scenarios of future environmental change. Chem. and microbial diversity were also pos. correlated, with dissolved org. matter having stronger effects on microbes than vice versa. Under our exptl. scenarios that increased sediment org. matter from 5 to 25% or darkened overlying waters by 2.5 times, the resulting increases in chemodiversity could increase greenhouse gas concns. in lake sediments by an av. of 1.5 to 2.7 times, when all of the other effects of litterfall and water color were considered. Our results open a major new avenue for research in aquatic ecosystems by exposing connections between chem. and microbial diversity and their implications for the global carbon cycle in greater detail than ever before.
27Tanentzap，AJ;惠誉，A.;奥兰，C.;埃米尔森，EJ S.;亚基莫维奇，KM;奥斯特霍尔茨，H.;Dittmar， T.淡水中的化学和微生物多样性协同变化影响生态系统功能。美国科学院院刊 2019， 116 （49）， 24689– 24695， DOI： 10.1073/pnas.1904896116 - 28Judd, K. E.; Crump, B. C.; Kling, G. W. Variation in dissolved organic matter controls bacterial production and community composition. EcologyIF 4.8SCIEJCI 1.3Q1环境科学与生态学2区Top2006, 87 (8), 2068– 2079, DOI: 10.1890/0012-9658(2006)87[2068:VIDOMC]2.0.CO;2 Google Scholar Google 学术搜索28https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A280%3ADC%252BD28rhtl2gsg%253D%253D&md5=40a3ee97588aeb824b803be4f9437133Variation in dissolved organic matter controls bacterial production and community compositionJudd Kristin E; Crump Byron C; Kling George WEcology (2006), 87 (8), 2068-79 ISSN:0012-9658.An ongoing debate in ecology revolves around how species composition and ecosystem function are related. To address the mechanistic controls of this relationship, we manipulated the composition of dissolved organic matter (DOM) fed to aquatic bacteria to determine effects on both bacterial activity and community composition. Sites along terrestrial to aquatic flow paths were chosen to simulate movement of DOM through catchments, and DOM was fed to downslope and control bacterial communities. Bacterial production was measured, and DOM chemistry and bacterial community composition (using denaturing gradient gel electrophoresis of 16S rRNA genes) were characterized following incubations. Bacterial production, dissolved organic carbon (DOC)-specific bacterial production, and DOC consumption were greatest in mesocosms fed soil water DOM; soil water DOM enhanced lake and stream bacterial production by 320-670% relative to lake and stream controls. Stream DOM added to lake bacteria depressed bacterial production relative to lake controls in the early season (-78%) but not the mid-season experiment. Addition of upslope DOM to stream and lake bacterial communities resulted in significant changes in bacterial community composition relative to controls. In four of five DOM treatments, the bacterial community composition converged to the DOM source community regardless of the initial inoculum. These results demonstrate that shifts in the supply of natural DOM were followed by changes in both bacterial production and community composition, suggesting that changes in function are likely predicated on at least an initial change in the community composition. The results indicate that variation in DOM composition of soil and surface waters influences bacterial community dynamics and controls rates of carbon processing in set patterns across the landscape.
28贾德，K.E.;克伦普，不列颠哥伦比亚省;Kling， G. W.溶解有机物的变化控制细菌的产生和群落组成。生态学2006， 87 （8）， 2068– 2079， DOI： 10.1890/0012-9658（2006）87 [2068：VIDOMC]2.0.CO;2 - 29Logue, J. B.; Stedmon, C. A.; Kellerman, A. M.; Nielsen, N. J.; Andersson, A. F.; Laudon, H.; Lindstrom, E. S.; Kritzberg, E. S. Experimental insights into the importance of aquatic bacterial community composition to the degradation of dissolved organic matter. ISME J.IF 11.0SCIEJCI 2.59Q1环境科学与生态学1区Top2016, 10 (3), 533– 545, DOI: 10.1038/ismej.2015.131 Google Scholar Google 学术搜索29https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC28XjtFKrsb0%253D&md5=6b5000920df98fcaea68d8158f5886a7Experimental insights into the importance of aquatic bacterial community composition to the degradation of dissolved organic matterLogue, Jurg B.; Stedmon, Colin A.; Kellerman, Anne M.; Nielsen, Nikoline J.; Andersson, Anders F.; Laudon, Hjalmar; Lindstroem, Eva S.; Kritzberg, Emma S.ISME Journal (2016), 10 (3), 533-545CODEN: IJSOCF; ISSN:1751-7362. (Nature Publishing Group)Bacteria play a central role in the cycling of carbon, yet our understanding of the relationship between the taxonomic compn. and the degrdn. of dissolved org. matter (DOM) is still poor. In this exptl. study, we were able to demonstrate a direct link between community compn. and ecosystem functioning in that differently structured aquatic bacterial communities differed in their degrdn. of terrestrially derived DOM. Although the same amt. of carbon was processed, both the temporal pattern of degrdn. and the compds. degraded differed among communities. We, moreover, uncovered that low-mol.-wt. carbon was available to all communities for utilization, whereas the ability to degrade carbon of greater mol. wt. was a trait less widely distributed. Finally, whereas the degrdn. of either low- or high-mol.-wt. carbon was not restricted to a single phylogenetic clade, our results illustrate that bacterial taxa of similar phylogenetic classification differed substantially in their assocn. with the degrdn. of DOM compds. Applying techniques that capture the diversity and complexity of both bacterial communities and DOM, our study provides new insight into how the structure of bacterial communities may affect processes of biogeochem. significance.
29洛格，J.B.;斯特德蒙，CA;凯勒曼，AM;尼尔森，新泽西州;安德森，AF;劳登，H.;林德斯特罗姆，ES;Kritzberg， E. S.对水生细菌群落组成对溶解有机物降解的重要性的实验见解。ISME J.2016， 10 （3）， 533– 545， DOI： 10.1038/ismej.2015.131 - 30Kujawinski, E. B. The impact of microbial metabolism on marine dissolved organic matter. Annu. Rev. Mar. Sci.IF 17.3SCIEJCI 2.47Q1地球科学1区Top2011, 3, 567– 599, DOI: 10.1146/annurev-marine-120308-081003 Google Scholar Google 学术搜索30https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A280%3ADC%252BC3M3gtlKrtQ%253D%253D&md5=f7bd65b5ad6db4014b202d175dcb6f89The impact of microbial metabolism on marine dissolved organic matterKujawinski Elizabeth BAnnual review of marine science (2011), 3 (), 567-99 ISSN:1941-1405.Microbes mediate global biogeochemical cycles through their metabolism, and all metabolic processes begin with the interaction between the microbial cell wall or membrane and the external environment. For all heterotrophs and many autotrophs, critical growth substrates and factors are present within the dilute and heterogeneous mixture of compounds that constitutes dissolved organic matter (DOM). In short, the microbe-molecule interaction is one of the fundamental reactions within the global carbon cycle. Here, I summarize recent findings from studies that examine DOM-microbe interactions from either the DOM perspective (organic geochemistry) or the microbe perspective (microbial ecology). Gaps in our knowledge are highlighted and future integrative research directions are proposed.
30Kujawinski， E. B.微生物代谢对海洋溶解有机物的影响。年。Rev. Mar. Sci.2011， 3， 567– 599， DOI： 10.1146/annurev-marine-120308-081003 - 31Osterholz, H.; Singer, G.; Wemheuer, B.; Daniel, R.; Simon, M.; Niggemann, J.; Dittmar, T. Deciphering associations between dissolved organic molecules and bacterial communities in a pelagic marine system. ISME J.IF 11.0SCIEJCI 2.59Q1环境科学与生态学1区Top2016, 10 (7), 1717– 1730, DOI: 10.1038/ismej.2015.231 Google Scholar Google 学术搜索31https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC28XhtVahu7fN&md5=253c21d9b747758f1b6733dd9f721a3eDeciphering associations between dissolved organic molecules and bacterial communities in a pelagic marine systemOsterholz, Helena; Singer, Gabriel; Wemheuer, Bernd; Daniel, Rolf; Simon, Meinhard; Niggemann, Jutta; Dittmar, ThorstenISME Journal (2016), 10 (7), 1717-1730CODEN: IJSOCF; ISSN:1751-7362. (Nature Publishing Group)Dissolved org. matter (DOM) is the main substrate and energy source for heterotrophic bacterioplankton. To understand the interactions between DOM and the bacterial community (BC), it is important to identify the key factors on both sides in detail, chem. distinct moieties in DOM and the various bacterial taxa. Next-generation sequencing facilitates the classification of millions of reads of environmental DNA and RNA amplicons and ultrahigh-resoln. mass spectrometry yields up to 10 000 DOM mol. formulas in a marine water sample. Linking this detailed biol. and chem. information is a crucial first step toward a mechanistic understanding of the role of microorganisms in the marine carbon cycle. In this study, we interpreted the complex microbiol. and mol. information via a novel combination of multivariate statistics. We were able to reveal distinct relationships between the key factors of org. matter cycling along a latitudinal transect across the North Sea. Total BC and DOM compn. were mainly driven by mixing of distinct water masses and presumably retain their resp. terrigenous imprint on similar timescales on their way through the North Sea. The active microbial community, however, was rather influenced by local events and correlated with specific DOM mol. formulas indicative of compds. that are easily degradable. These trends were most pronounced on the highest resolved level, i.e., operationally defined 'species', reflecting the functional diversity of microorganisms at high taxonomic resoln. Sequence data were deposited inthe Sequence Read Archive (SRA) of the National Center for Biotechnol. Information (NCBI) under the accession no. SRA082674.
31奥斯特霍尔茨，H.;歌手，G.;Wemheuer，B.;丹尼尔，R.;西蒙，M.;尼格曼，J.;Dittmar， T.破译中上层海洋系统中溶解有机分子与细菌群落之间的关联。ISME J.2016， 10 （7）， 1717– 1730， DOI： 10.1038/ismej.2015.231 - 32Bader, H. Determination of ozone in water by the indigo method: A submitted standard method. Ozone: Sci. Eng.IF 2.7SCIEJCI 0.32Q3环境科学与生态学4区1982, 4 (4), 169– 176, DOI: 10.1080/01919518208550955 Google Scholar Google 学术搜索32https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADyaL3sXksVeitLg%253D&md5=f077fd7064dc297741a9c0c09f725531Determination of ozone in water by the indigo method; a submitted standard methodBader, H.; Hoigne, J.Ozone: Science & Engineering (1982), 4 (4), 169-76CODEN: OZSEDS; ISSN:0191-9512.A selective and simple method for the detn. of O3, as formulated for the new Swiss Std. Methods for drinking water anal., is presented. O3 rapidly and stoichiometrically decolorizes tri-K indigo trisulfonate [67627-18-3] in acidic soln. The decrease in absorbance at 600 nm is linear with O3 residual and is 0.42 ± 0.01/cm per mg/L. The limits of detection are 2 μg μg/L for an instrumental and 10 mg/L for a visual field method.
32Bader， H.用靛蓝法测定水中的臭氧：提交的标准方法。臭氧： Sci. Eng.1982， 4 （4）， 169– 176， DOI： 10.1080/01919518208550955 - 33Dittmar, T.; Koch, B.; Hertkorn, N.; Kattner, G. A simple and efficient method for the solid-phase extraction of dissolved organic matter (SPE-DOM) from seawater. Limnol. Oceanogr.: MethodsIF 2.7SCIEJCI 0.84Q2地球科学3区2008, 6, 230– 235, DOI: 10.4319/lom.2008.6.230 Google Scholar Google 学术搜索33https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BD1cXhtlOnt7jI&md5=3f114d54f73464b3c5dc217c5fd7790eA simple and efficient method for the solid-phase extraction of dissolved organic matter (SPE-DOM) from seawaterDittmar, Thorsten; Koch, Boris; Hertkorn, Norbert; Kattner, GerhardLimnology and Oceanography: Methods (2008), 6 (June), 230-235CODEN: LOMIBY; ISSN:1541-5856. (American Society of Limnology and Oceanography)A simple protocol is presented for the solid-phase extn. of dissolved org. matter (SPE-DOM) from seawater using com. prepacked cartridges. The method does not require major instrumentation and can be performed in the field. Modified styrene divinyl benzene polymer type sorbents (Varian PPL and ENV) and sorbents of a silica structure bonded with different hydrocarbon chains (Varian C8, C18, C18OH, and C18EWP) were considered. Except for C18OH, which heavily contaminated the samples, none of the sorbents leached significant amts. of dissolved org. carbon (DOC) or nitrogen (DON). Samples from the North Brazil shelf with strong mixing gradients of terrigenous and marine DOM were used to compare the various sorbents. PPL was the most efficient-on av., 62% of DOC was recovered as salt-free exts. C18 was found to be most efficient among the silica-based sorbents, but it showed only two-thirds of the extn. efficiency of PPL. As indicated by [1H]NMR, C/N, and δ13C analyses, PPL extd. a more representative proportion of DOM than C18. Therefore, PPL was used for comparative studies in the Gulf of Mexico and Antarctica. From brackish marsh and river waters, 65% and 62% of total DOC, resp., could be extd. For purely marine DOM in Antarctica and the deep sea, the extn. efficiency was lower (43% on av.). The efficiency of the new method to isolate marine DOM is better than or similar to highly laborious methods. A further advantage is the complete desalination of the sample. The isolation of a major DOM fraction, which is salt-free, offers many possibilities to further characterize DOM by advanced anal. techniques.
33迪特玛，T.;科赫，B.;牧谷物，N.;Kattner， G.一种简单有效的海水中溶解有机物固相萃取方法（SPE-DOM）。利姆诺尔。Oceanogr.： 方法2008， 6， 230– 235， DOI： 10.4319/lom.2008.6.230 - 34Li, F.; Tang, S.; Lv, J.; He, A.; Wang, Y.; Liu, S.; Cao, H.; Zhao, L.; Wang, Y.; Jiang, G. Molecular-scale investigation on the formation of brown carbon aerosol via iron-phenolic compound reactions in the dark. Environ. Sci. Technol.IF 11.4SCIEJCI 1.44Q1环境科学与生态学1区Top2023, 57 (30), 11173– 11184, DOI: 10.1021/acs.est.3c04263 Google Scholar Google 学术搜索There is no corresponding record for this reference.
34李，F.;唐，S.;吕J.;他，A.;王彦;刘，S.;曹浩;赵玲玲;王彦;江， G.黑暗中铁酚化合物反应形成褐碳气溶胶的分子尺度研究.环境。科学技术.2023， 57 （30）， 11173– 11184， DOI： 10.1021/acs.est.3c04263 - 35Zherebker, A.; Shirshin, E.; Rubekina, A.; Kharybin, O.; Kononikhin, A.; Kulikova, N. A.; Zaitsev, K. V.; Roznyatovsky, V. A.; Grishin, Y. K.; Perminova, I. V.; Nikolaev, E. N. Optical properties of soil dissolved organic matter are related to acidic functions of its components as revealed by fractionation, selective deuteromethylation, and ultrahigh resolution mass spectrometry. Environ. Sci. Technol.IF 11.4SCIEJCI 1.44Q1环境科学与生态学1区Top2020, 54 (5), 2667– 2677, DOI: 10.1021/acs.est.9b05298 Google Scholar Google 学术搜索35https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BB3cXislartb0%253D&md5=b4eb098cd023482ec11f33b75fd25fa6Optical Properties of Soil Dissolved Organic Matter Are Related to Acidic Functions of Its Components as Revealed by Fractionation, Selective Deuteromethylation, and Ultrahigh Resolution Mass SpectrometryZherebker, Alexander; Shirshin, Evgeny; Rubekina, Anna; Kharybin, Oleg; Kononikhin, Alexey; Kulikova, Natalia A.; Zaitsev, Kirill V.; Roznyatovsky, Vitaliy A.; Grishin, Yuri K.; Perminova, Irina V.; Nikolaev, Evgeny N.Environmental Science & Technology (2020), 54 (5), 2667-2677CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)The goal of this study was to establish a relationship between the optical properties of soil dissolved org. matter (DOM) and acidic functions carried out by its individual constituents. We obtained 12 fractions of DOM samples using sequential solid phase extn. on nonionic sorbent at steadily lowered pH values: 7, 5, 3, 2, which correspond to low bounds of pKa values of phenols, aliph., and arom. carboxylic acids, and ketoacids. The structural studies were conducted with the use of NMR and selective deuteromethylation of isolated fractions coupled to ultrahigh resoln. mass spectrometry. First, a gradual shift of mol. compns. was obsd. from reduced components to arom. oxidized compds. isolated at pH 7 and 2, resp. Changes in mol. compns. were accompanied by a red shift of fluorescence spectra. Further application of deuteromethylation enabled us to distinguish DOM constituents with different amts. of carboxylic groups. Moreover, identification of structural isomers in a single DOM sample was achieved. Statistical anal. revealed that red shift of fluorescence is facilitated by the increase of a contribution of arom. poly(carboxylic acid)s with high conjugation lengths. Addnl., anal. of the labeled fractionated permafrost thaw DOM directly showed carboxyl-rich alicyclic mols., while the same components from lower-latitude DOM were assigned to lignin-like species.
35泽列布克，A.;希尔辛，E.;鲁贝金娜，A.;哈里宾，O.;科诺尼欣，A.;库利科娃，N.A.;扎伊采夫，K.V.;罗兹尼亚托夫斯基，V.A.;格里申，Y.K.;佩尔米诺娃，I.V.;Nikolaev， E. N.土壤溶解有机物的光学特性与其组分的酸性功能有关，如分馏、选择性去甲基化和超高分辨率质谱法所揭示的那样。环境。科学技术.2020， 54 （5）， 2667– 2677， DOI： 10.1021/acs.est.9b05298 - 36Lv, J. T.; Zhang, S. Z.; Wang, S. S.; Luo, L.; Cao, D.; Christie, P. Molecular-scale investigation with ESI-FT-ICR-MS on fractionation of dissolved organic matter induced by adsorption on iron oxyhydroxides. Environ. Sci. Technol.IF 11.4SCIEJCI 1.44Q1环境科学与生态学1区Top2016, 50 (5), 2328– 2336, DOI: 10.1021/acs.est.5b04996 Google Scholar Google 学术搜索36https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC28XhsVymsrg%253D&md5=41055937d3e93d140dfa0e258cbd8fa5Molecular-Scale Investigation with ESI-FT-ICR-MS on Fractionation of Dissolved Organic Matter Induced by Adsorption on Iron OxyhydroxidesLv, Jitao; Zhang, Shuzhen; Wang, Songshan; Luo, Lei; Cao, Dong; Christie, PeterEnvironmental Science & Technology (2016), 50 (5), 2328-2336CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)Adsorption by minerals is a common geochem. process of dissolved org. matter (DOM) which may induce fractionation of DOM at the mineral-water interface. We examine the mol. fractionation of DOM induced by adsorption onto 3 common iron oxyhydroxides using electrospray ionization coupled with Fourier-transform ion cyclotron resonance mass spectrometry (ESI-FT-ICR-MS). Ferrihydrite exhibited higher affinity to DOM and induced more pronounced mol. fractionation of DOM than did goethite or lepidocrocite. High mol. wt. (>500 Da) compds. and compds. high in unsatn. or rich in O including polycyclic aroms., polyphenols and carboxylic compds. had higher affinity to Fe oxyhydroxides and esp. to ferrihydrite. Low mol. wt. compds. and compds. low in unsatn. or contg. few oxygenated groups (mainly alcs. and ethers) were preferentially maintained in soln. This study confirms that the double bond equivalence and the no. of O atoms are valuable parameters indicating the selective fractionation of DOM at mineral and water interfaces. The results provide important information for further understanding the behavior of DOM in the natural environment.
36Lv，J.T.;张S.Z.;王淑娟;罗玖;曹，D.;Christie， P.使用ESI-FT-ICR-MS进行分子尺度研究，研究吸附在氢氧化铁上诱导的溶解有机物的分馏。环境。科学技术.2016， 50 （5）， 2328– 2336， DOI： 10.1021/acs.est.5b04996 - 37Yu, S.; Lv, J.; Jiang, L.; Geng, P.; Cao, D.; Wang, Y. Changes of soil dissolved organic matter and its relationship with microbial community along the Hailuogou Glacier forefield chronosequence. Environ. Sci. Technol.IF 11.4SCIEJCI 1.44Q1环境科学与生态学1区Top2023, 57 (9), 4027– 4038, DOI: 10.1021/acs.est.2c08855 Google Scholar Google 学术搜索37https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BB3sXjsF2ku70%253D&md5=2027aea4128a32032070ee402ce859cdChanges of Soil Dissolved Organic Matter and Its Relationship with Microbial Community along the Hailuogou Glacier Forefield ChronosequenceYu, Shiyang; Lv, Jitao; Jiang, Lu; Geng, Pengyu; Cao, Dong; Wang, YaweiEnvironmental Science & Technology (2023), 57 (9), 4027-4038CODEN: ESTHAG; ISSN:1520-5851. (American Chemical Society)Glacier-retreated areas are ideal areas to study soil biogeochem. processes during vegetation succession, because of the limited effect of other environmental and climatic factors. In this study, the changes of soil dissolved org. matter (DOM) and its relationship with microbial communities along the Hailuogou Glacier forefield chronosequence were investigated. Both microbial diversity and DOM mol. chemodiversity recovered rapidly at the initial stage, indicating the pioneering role of microorganisms in soil formation and development. The chem. stability of soil org. matter enhanced with vegetation succession due to the retaining of compds. with high oxidn. state and aromaticity. The mol. compn. of DOM affected microbial communities, while microorganisms tended to utilize labile components to form refractory components. This complex relationship network between microorganisms and DOM components played an important role in the development of soil org. matter as well as the formation of stable soil carbon pool in glacier-retreated areas.
37余，S.;吕J.;江，L.;耿，P.;曹，D.;Wang， Y.海螺沟冰川前场年代序列土壤溶解有机质变化及其与微生物群落的关系.环境。科学技术.2023， 57 （9）， 4027– 4038， DOI： 10.1021/acs.est.2c08855 - 38Lv, J.; Miao, Y.; Huang, Z.; Han, R.; Zhang, S. Facet-mediated adsorption and molecular fractionation of humic substances on hematite surfaces. Environ. Sci. Technol.IF 11.4SCIEJCI 1.44Q1环境科学与生态学1区Top2018, 52 (20), 11660– 11669, DOI: 10.1021/acs.est.8b03940 Google Scholar Google 学术搜索38https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC1cXhslantbzF&md5=a7f01e37d9f34127ca60d39cdd847990Facet-Mediated Adsorption and Molecular Fractionation of Humic Substances on Hematite SurfacesLv, Jitao; Miao, Yuexia; Huang, Zaoquan; Han, Ruixia; Zhang, ShuzhenEnvironmental Science & Technology (2018), 52 (20), 11660-11669CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)Interactions between dissolved org. matter (DOM) and iron oxyhydroxides have important environmental and geochem. implications. The present study employed two hematite nanocrystals to investigate the adsorption and mol. fractionation of two typical humic substances (HSs) using electrospray ionization coupled with Fourier transform ion cyclotron resonance mass spectrometry (ESI-FT-ICR-MS). Hematite with a predominant exposure of {100} facets induced more pronounced adsorption and mol. fractionation of HSs than {001} facets, indicating that the interfacial adsorptive fractionation process of HSs was mediated by exposed facets of hematite. Further exploration of the surface OH groups of the two hematite nanocrystals confirms that the facet-mediated mol. fractionation of HSs was attributable to the abundance of singly iron-atom coordinated -OH sites on the hematite surfaces. Mols. with a high oxidn. state and high aromaticity such as oxidized black carbon, polyphenol-like, and tannic-like compds. preferentially formed ligand-exchange complexes with singly coordinated -OH groups on the hematite surfaces, inducing the selective binding and mol. fractionation of HSs at the mineral-water interface. These results demonstrate that singly iron-atom coordinated -OH sites det. DOM adsorption and mediate mol. fractionation on hematite surfaces, and this contributes substantially to our understanding of the mol. mechanisms of iron oxyhydroxide-mediated mol. exchange of DOM in soils and/or sediments.
38Lv，J.;苗，Y.;黄志强;韩，R.;Zhang， S.Facet介导的赤铁矿表面腐殖质物质的吸附和分子分馏.环境。科学技术.2018， 52 （20）， 11660– 11669， DOI： 10.1021/acs.est.8b03940 - 39Koch, B. P.; Dittmar, T.; Witt, M.; Kattner, G. Fundamentals of molecular formula assignment to ultrahigh resolution mass data of natural organic matter. Anal. Chem.IF 7.4SCIEJCI 1.71Q1化学1区Top2007, 79 (4), 1758– 1763, DOI: 10.1021/ac061949s Google Scholar Google 学术搜索39https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BD2sXjtVahtg%253D%253D&md5=b296c368a5fbeb290a77e549ec58487bFundamentals of molecular formula assignment to ultrahigh resolution mass data of natural organic matterKoch, Boris P.; Dittmar, Thorsten; Witt, Matthias; Kattner, GerhardAnalytical Chemistry (2007), 79 (4), 1758-1763CODEN: ANCHAM; ISSN:0003-2700. (American Chemical Society)Ultrahigh-resoln. mass spectrometry via the Fourier transform ICR technique (FT-ICR-MS) allows the identification of thousands of different mol. formulas in natural org. matter and petroleum samples. Mol. formula assignment from mass data is most crit. and time-consuming for these samples, and in many cases, several formulas can be detd. for the same mol. mass. Therefore, automated procedures are required for an efficient exploitation of the extensive data sets. Here, the authors revise statements in a recent publication, which might result in a misleading impression about the authors' approach of formula assignment in a previous work. The authors also summarize and categorize existing procedures for formula assignment. The authors propose new techniques, which are suitable to be implemented in automated evaluation software. The homologous series approach is extended toward a building block approach that can be applied as a new exclusion criterion for incorrect formula assignments. The examn. of stable isotope ratios of individual mols. in natural org. matter can be applied as an addnl. and intrinsic evaluation for calcd. mol. formulas.
39科赫，BP;迪特玛，T.;威特，M.;Kattner， G.天然有机物超高分辨率质量数据分子式分配的基础。分析化学.2007， 79 （4）， 1758– 1763， DOI： 10.1021/ac061949s - 40Sun, K.; Han, L. F.; Yang, Y.; Xia, X. H.; Yang, Z. F.; Wu, F. C.; Li, F. B.; Feng, Y. F.; Xing, B. S. Application of hydrochar altered soil microbial community composition and the molecular structure of native soil organic carbon in a paddy soil. Environ. Sci. Technol.IF 11.4SCIEJCI 1.44Q1环境科学与生态学1区Top2020, 54 (5), 2715– 2725, DOI: 10.1021/acs.est.9b05864 Google Scholar Google 学术搜索40https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BB3cXitFejsrY%253D&md5=a50ee46c2ba85eb40d5b47850626c3f8Application of Hydrochar Altered Soil Microbial Community Composition and the Molecular Structure of Native Soil Organic Carbon in a Paddy SoilSun, Ke; Han, Lanfang; Yang, Yan; Xia, Xinghui; Yang, Zhifeng; Wu, Fengchang; Li, Fangbai; Feng, Yanfang; Xing, BaoshanEnvironmental Science & Technology (2020), 54 (5), 2715-2725CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)The benefits and disadvantages of hydrochar incorporation into soil have been heavily researched. However, the effect of hydrochar application on the soil microbial communities and the mol. structure of native soil org. carbon (SOC) has not been thoroughly elucidated. This study conducted an incubation expt. at 25°C for 135 days using a soil column with 0.5 and 1.5% hydrochar-amended paddy soil to explore the interconnections between changes in soil properties and microbial communities and shifts in native SOC structure using electrospray ionization Fourier transform ion cyclotron resonance mass spectrometry (ESI-FT-ICR-MS) and NMR after hydrochar application. Hydrochar addn. decreased the labile SOC fraction by 15.6-33.6% and increased the stable SOC fraction by 10.3-27.0%. These effects were significantly stronger for 1.5% hydrochar-treated soil. Addnl., hydrochar addn. induced the native SOC with 1.0-3.0% more carbon and 6.0-13.0% higher mol. wt. The SOC in hydrochar-amended soil contained more arom. compds. but fewer carbohydrates and lower polarity. This was resulted by a statistically significant redn. in Sphingobacterium, which was active in polycyclic arom. hydrocarbon degrdn., and an increase in Flavobacterium, Anaerolinea, Penicillium, and Acremonium, which were the efficient decomposers of labile SOC. These findings will help elucidate the potential influence of hydrochar on the carbon biogeochem. cycle in the soil.
40孙，K.;韩，L.F.;杨，Y.;夏旭华;杨志芳;吴，F.C.;李，F.B.;冯永芳;Xing， B. S.水炭改变水稻土壤微生物群落组成及天然土壤有机碳分子结构的应用.环境。科学技术.2020， 54 （5）， 2715– 2725， DOI： 10.1021/acs.est.9b05864 - 41Koch, B. P.; Dittmar, T. From mass to structure: An aromaticity index for high-resolution mass data of natural organic matter. Rapid Commun. Mass Spectrom.IF 2.0SCIEJCI 0.65Q3化学3区2006, 20 (5), 926– 932, DOI: 10.1002/rcm.2386 Google Scholar Google 学术搜索41https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BD28XitlGgs74%253D&md5=86bf95387b3e6f752481d4f026cbd184From mass to structure: an aromaticity index for high-resolution mass data of natural organic matterKoch, B. P.; Dittmar, T.Rapid Communications in Mass Spectrometry (2005), 20 (5), 926-932CODEN: RCMSEF; ISSN:0951-4198. (John Wiley & Sons Ltd.)Recent progress in Fourier transform ion cyclotron resonance mass spectrometry (FTICRMS) has provided extensive mol. mass data for complex natural org. matter (NOM). Structural information can be deduced solely from the mol. masses for ions with extreme mol. element ratios, in particular low H/C ratios, which are abundant in thermally altered NOM (e.g. black carbon). In this communication we propose a general aromaticity index (AI) and two threshold values as unequivocal criteria for the existence of either arom. (AI > 0.5) or condensed arom. structures (AI ≥ 0.67) in NOM. AI can be calcd. from mol. formulas which are derived from exact mol. masses of naturally occurring compds. contg. C, H, O, N, S and P, and is esp. useful for substances with arom. cores and few alkylations. In order to test the validity of our model index, AI is applied to FTICRMS data of a NOM deep-water sample from the Weddell Sea (Antarctica), a fulvic acid std., and an artificial dataset of all theor. possible mol. formulas. For graphical evaluation a ternary plot is suggested for four-dimensional data representation. The proposed aromaticity index is a step towards structural identification of NOM and the mol. identification of polyarom. hydrocarbons in the environment.
41科赫，BP;Dittmar， T.从质量到结构：天然有机物高分辨率质量数据的芳香指数。快速通信。质谱.2006， 20 （5）， 926– 932， DOI： 10.1002/rcm.2386 - 42Ding, Y.; Shi, Z. Q.; Ye, Q. T.; Liang, Y. Z.; Liu, M. Q.; Dang, Z.; Wang, Y. J.; Liu, C. X. Chemodiversity of soil dissolved organic matter. Environ. Sci. Technol.IF 11.4SCIEJCI 1.44Q1环境科学与生态学1区Top2020, 54 (10), 6174– 6184, DOI: 10.1021/acs.est.0c01136 Google Scholar Google 学术搜索42https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BB3cXntl2ku74%253D&md5=753cd5d70afbd947afb7d847cb39bc0aChemodiversity of Soil Dissolved Organic MatterDing, Yang; Shi, Zhenqing; Ye, Qianting; Liang, Yuzhen; Liu, Minqin; Dang, Zhi; Wang, Yujun; Liu, ChongxuanEnvironmental Science & Technology (2020), 54 (10), 6174-6184CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)Dissolved org. matter (DOM) plays a key role in many biogeochem. processes, but the drivers controlling the diversity of chem. compn. and properties of DOM mols. (chemodiversity) in soils are poorly understood. It has also been debated whether environmental conditions or intrinsic mol. properties control the accumulation and persistence of DOM due to the complexity of both mol. compn. of DOM and interactions between DOM and surrounding environments. Soil DOM samples were extd. from 33 soils collected from different regions of China, and we studied the effects of climate and soil properties on the chemodiversity of DOM across different regions of China, employing a combination of Fourier transform ICR mass spectrometry, optical spectroscopy, and statistical analyses. Despite the heterogeneity of soil samples and complex influencing factors, aridity and clay can account for the majority of the variations of DOM chem. compn. The finding implied that DOM chemodiversity is an ecosystem property closely related to the environment, and can be used in developing large-scale soil biogeochem. models for predicting C cycling in soils.
42丁，Y.;石志Q.;叶，Q.T.;梁玉璧;刘明问;邓，Z.;王玉杰;Liu， C. X.土壤溶解有机质的化学多样性.大约。Sci. Technol.2020， 54 （10）， 6174–6184， DOI： 10.1021/acs.est.0c01136 - 43Lawaetz, A. J.; Stedmon, C. A. Fluorescence intensity calibration using the Raman scatter peak of water. Appl. Spectrosc.IF 3.5SCIEJCI 0.91Q1化学3区2009, 63 (8), 936– 940, DOI: 10.1366/000370209788964548 Google Scholar Google 学术搜索43https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BD1MXhtVaht7fM&md5=9b276ac6eb08dda3e51c3f158d5c287eFluorescence intensity calibration using the Raman scatter peak of waterLawaetz, A. J.; Stedmon, C. A.Applied Spectroscopy (2009), 63 (8), 936-940CODEN: APSPA4; ISSN:0003-7028. (Society for Applied Spectroscopy)Fluorescence data of replicate samples obtained from different fluorescence spectrometers or by the same spectrometer but with different instrument settings can have great intensity differences. To compare such data an intensity calibration must be applied. Here we explain a simple calibration method for fluorescence intensity using only the integrated area of a water Raman peak. By applying this method to data from three different instruments, we show that it is possible to remove instrument-dependent intensity factors, and we present results on a unified scale of Raman units. The method presented is a rapid and simple approach suitable for routine measurements with no need for hazardous chems.
43拉瓦茨，AJ;Stedmon， C. A.使用水的拉曼散射峰进行荧光强度校准。应用光谱.2009， 63 （8）， 936– 940， DOI： 10.1366/000370209788964548 - 44Gong, J.; Liu, Y.; Sun, X. O3 and UV/O3 oxidation of organic constituents of biotreated municipal wastewater. Water Res.IF 12.8SCIEJCI 2.15Q1环境科学与生态学1区Top2008, 42 (4–5), 1238– 1244, DOI: 10.1016/j.watres.2007.09.020 Google Scholar Google 学术搜索44https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BD1cXhvFyrtL4%253D&md5=915943a456b48176f79ca420443bf2f8O3 and UV/O3 oxidation of organic constituents of biotreated municipal wastewaterGong, Jianli; Liu, Yongdi; Sun, XianboWater Research (2008), 42 (4-5), 1238-1244CODEN: WATRAG; ISSN:0043-1354. (Elsevier Ltd.)Dissolved org. matter (DOM) in the biotreated effluent of a municipal wastewater treatment plant was sepd. by XAD-8 and XAD-4 resins into four fractions: hydrophobic acids, non-acid hydrophobics, transphilics and hydrophilics. Ozonation with and without UV enhancement removed most UV-absorbing substances in the first 30 min achieving 78% and 63% redn. in UV254, resp.; the UV enhancement resulted in a greater redn. in dissolved org. carbon (DOC) (90% vs. 36%). Ozone reacted sequentially with arom. hydrophobics, transphilics, and then hydrophilics; however, under UV, it reacted with all four org. fractions simultaneously. Low-MW hydrophilics were the most abundant fraction in the ozone-treated effluent.
44龚，J.;刘彦;生物处理城市废水中有机成分的太阳、X.O 3 和 UV/O 3 氧化。水研究 2008， 42 （4–5）， 1238– 1244， DOI： 10.1016/j.watres.2007.09.020 - 45Ohno, T.; He, Z.; Sleighter, R. L.; Honeycutt, C. W.; Hatcher, P. G. Ultrahigh resolution mass spectrometry and indicator species analysis to identify marker components of soil- and plant biomass- derived organic matter fractions. Environ. Sci. Technol.IF 11.4SCIEJCI 1.44Q1环境科学与生态学1区Top2010, 44 (22), 8594– 8600, DOI: 10.1021/es101089t Google Scholar Google 学术搜索45https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC3cXhtlShs7rK&md5=d82e6c5d259208b4b53548c6928c4453Ultrahigh Resolution Mass Spectrometry and Indicator Species Analysis to Identify Marker Components of Soil- and Plant Biomass-Derived Organic Matter FractionsOhno, Tsutomu; He, Zhongqi; Sleighter, Rachel L.; Honeycutt, C. Wayne; Hatcher, Patrick G.Environmental Science & Technology (2010), 44 (22), 8594-8600CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)The chem. properties of org. matter affect important soil processes such as speciation, solubilization, and transport of plant nutrients and metals. This work uses ultrahigh resoln. electrospray ionization Fourier transform ion cyclotron resonance mass spectrometry to det. the mol. compn. of three org. matter fractions of soils and aq. exts. of crop biomass. Comparison of the van Krevelen plots allowed tracking the changes in org. matter with increasing humification. Aq. plant biomass exts. contain a diverse mixt. of lipids, proteins, and lignins. Soil aq. exts. were marked by increases in lignin and carbohydrate components and decrease in the protein component as compared to the plant ext. Refractory humic acid fractions were marked by decrease in the lignin component and increases in the lipid and condensed arom. components. The multivariate indicator species anal. was used to identify marker components of the four org. matter types investigated. The plant ext. group had 772 marker components compared to 237 for soil aq. ext., 92 for mobile humic acid, and 418 for calcium humic acid. This study demonstrates that ultrahigh resoln. mass spectrometry and multivariate methods can be used to identify marker components to gain a mol.-scale description and understanding of C dynamics.
45大野，T.;他，Z.;斯莱特，RL;霍尼卡特，CW;Hatcher， P. G.超高分辨率质谱和指示物物种分析，用于识别土壤和植物生物质衍生有机质组分的标记成分。环境。科学技术.2010， 44 （22）， 8594– 8600， DOI： 10.1021/es101089t - 46LaRowe, D. E.; Van Cappellen, P. Degradation of natural organic matter: A thermodynamic analysis. Geochim. Cosmochim. ActaIF 5.0SCIEJCI 1.52Q1地球科学1区Top2011, 75 (8), 2030– 2042, DOI: 10.1016/j.gca.2011.01.020 Google Scholar Google 学术搜索46https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC3MXjsVGhu78%253D&md5=3a0610f4c212fc480d02649866bfdffdDegradation of natural organic matter: A thermodynamic analysisLaRowe, Douglas E.; Van Cappellen, PhilippeGeochimica et Cosmochimica Acta (2011), 75 (8), 2030-2042CODEN: GCACAK; ISSN:0016-7037. (Elsevier B.V.)The oxidative degrdn. of org. matter is a key process in the biogeochem. functioning of the earth system. Quant. models of org. matter degrdn. are therefore essential for understanding the chem. state and evolution of the Earth's near-surface environment, and to forecast the biogeochem. consequences of ongoing regional and global change. The complex nature of biol. produced org. matter represents a major obstacle to the development of such models, however. The authors compare the energetics of the oxidative degrdn. of a large no. of naturally occurring org. compds. By relating the Gibbs energies of half reactions describing the complete mineralization of the compds. to their av. nominal carbon oxidn. state, it becomes possible to est. the energetic potential of the compds. based on major element (C, H, N, O, P, S) ratios. The new energetic description of org. matter can be combined with bioenergetic theory to rationalize obsd. patterns in the decompn. of natural org. matter. For example, the persistence of cell membrane derived compds. and complex orgs. in anoxic settings is consistent with their limited catabolic potential under these environmental conditions. The proposed approach opens the way to include the thermodn. properties of org. compds. in kinetic models of org. matter degrdn.
46拉罗，D.E.;Van Cappellen， P.天然有机物的降解：热力学分析。Geochim。科斯莫奇姆。学报2011， 75 （8）， 2030– 2042， DOI： 10.1016/j.gca.2011.01.020 - 47Ribeirinho-Soares, S.; Moreira, N. F. F.; Graca, C.; Pereira, M. F. R.; Silva, A. M. T.; Nunes, O. C. Overgrowth control of potentially hazardous bacteria during storage of ozone treated wastewater through natural competition. Water Res.IF 12.8SCIEJCI 2.15Q1环境科学与生态学1区Top2022, 209, 117932, DOI: 10.1016/j.watres.2021.117932 Google Scholar Google 学术搜索47https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BB3MXislWku77M&md5=d2a523efc46f70766df13794f91f3681Overgrowth control of potentially hazardous bacteria during storage of ozone treated wastewater through natural competitionRibeirinho-Soares, Sara; Moreira, Nuno F. F.; Graca, Catia; Pereira, M. Fernando R.; Silva, Adrian M. T.; Nunes, Olga C.Water Research (2022), 209 (), 117932CODEN: WATRAG; ISSN:0043-1354. (Elsevier Ltd.)Improving the chem. and biol. quality of treated wastewater is particularly important in world regions under water stress. In these regions, reutilization of wastewater is seen as an alternative to reduce water demand, particularly for agriculture irrigation. In a reuse scenario, the treated wastewater must have enough quality to avoid chem. and biol. contamination of the receiving environment. Ozonation is among the technologies available to efficiently remove org. micropollutants and disinfect secondary effluents, being implemented in full-scale urban wastewater treatment plants worldwide. However, previous studies demonstrated that storage of ozone treated wastewater promoted the overgrowth of potentially harmful bacteria, putting at risk its reutilization, given for instance the possibility of contaminating the food-chain. Therefore, this study was designed to assess the potential beneficial role of inoculation of ozone treated wastewater with a diverse bacterial community during storage, for the control of the overgrowth of potentially hazardous bacteria, through bacterial competition. To achieve this goal, ozone treated wastewater (TWW) was dild. with river water (RW) in the same proportion, and the resulting bacterial community (RW+TWW) was compared to that of undiluted TWW over 7 days storage. As hypothesized, in contrast to TWW, where dominance of Beta- and Gammaproteobacteria, namely Pseudomonas spp. and Acinetobacter spp., was obsd. upon storage for 7 days, the bacterial communities of the dild. samples (RW+TWW) were diverse, resembling those of RW. Moreover, given the high abundance of antibiotic resistance genes in RW, the concn. of these genes in RW+TWW did not differ from that of the non-ozonated controls (WW, RW and RW+WW) over the storage period. These results highlight the necessity of finding a suitable pristine diverse bacterial community to be used in the future to compete with bacteria surviving ozonation, to prevent reactivation of undesirable bacteria during storage of treated wastewater.
47里贝里尼奥-苏亚雷斯;莫雷拉，NFF;格拉卡，C.;佩雷拉，MFR;席尔瓦，AMT;Nunes， O. C.通过自然竞争在臭氧处理废水储存过程中对潜在有害细菌的过度生长控制。水研究 2022， 209， 117932， DOI： 10.1016/j.watres.2021.117932 - 48Rehman, Z. U.; Ali, M.; Iftikhar, H.; Leiknes, T. Genome-resolved metagenomic analysis reveals roles of microbial community members in full-scale seawater reverse osmosis plant. Water Res.IF 12.8SCIEJCI 2.15Q1环境科学与生态学1区Top2019, 149, 263– 271, DOI: 10.1016/j.watres.2018.11.012 Google Scholar Google 学术搜索There is no corresponding record for this reference.
48拉赫曼，Z.U.;阿里，M.;伊夫蒂哈尔，H.;基因组分辨的宏基因组分析揭示了微生物群落成员在全尺寸海水反渗透工厂中的作用。水研究 2019， 149， 263– 271， DOI： 10.1016/j.watres.2018.11.012 - 49Wang, H.; Zhang, C.; Wang, Y.-N.; Sun, Y.; Fu, Y.; Gong, Z.; Liu, K. Simultaneous degradation of refractory organics, antibiotics and antibiotic resistance genes from landfill leachate concentrate by GAC/O3. J. Cleaner Prod.IF 11.1SCIEJCI 1.53Q1环境科学与生态学1区Top2022, 380, 135016, DOI: 10.1016/j.jclepro.2022.135016 Google Scholar Google 学术搜索There is no corresponding record for this reference.
49王斌;张，C.;王彦娥;孙，Y.;傅彦;龚，Z.;Liu， K.GAC/O 3 对垃圾渗滤液浓缩物中难治性有机物、抗生素和抗生素抗性基因的同步降解.J. Cleaner Prod.2022， 380， 135016， DOI： 10.1016/j.jclepro.2022.135016 - 50Tadonléké, R. D. Strong coupling between natural Planctomycetes and changes in the quality of dissolved organic matter in freshwater samples. FEMS Microbiol. Ecol.IF 4.2SCIEJCI 0.8Q2生物学3区2007, 59 (3), 543– 555, DOI: 10.1111/j.1574-6941.2006.00222.x Google Scholar Google 学术搜索There is no corresponding record for this reference.
50Tadonléké， R. D.天然浮游菌与淡水样品中溶解有机物质量变化之间的强耦合。FEMS微生物。生态学2007， 59 （3）， 543– 555， DOI： 10.1111/j.1574-6941.2006.00222.x - 51Nichols, G. L.; McLauchlin, J. Microbiology and the investigation of waterborne outbreaks: The use of Cryptosporidium typing in the investigation of waterborne disease. In Drinking Water and Infectious Disease: Establishing the Links; CRC Press, 2002, pp 87– 95. DOI: 10.1201/9781420040524.ch8 .Google Scholar Google 学术搜索There is no corresponding record for this reference.
51尼科尔斯，GL;McLauchlin， J.微生物学和水传播暴发的调查：隐孢子虫分型在水传播疾病调查中的应用。在饮用水和传染病：建立联系;CRC出版社，2002年，第87-95页。DOI： 10.1201/9781420040524.ch8 . - 52Lau, H. Y.; Ashbolt, N. J. The role of biofilms and protozoa in Legionella pathogenesis: Implications for drinking water. J. Appl. Microbiol.IF 4.0SCIEJCI 0.68Q2生物学3区2009, 107 (2), 368– 378, DOI: 10.1111/j.1365-2672.2009.04208.x Google Scholar Google 学术搜索52https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A280%3ADC%252BD1MvptFWjtw%253D%253D&md5=c74d388e5e2f29221200d8b4ac872b8cThe role of biofilms and protozoa in Legionella pathogenesis: implications for drinking waterLau H Y; Ashbolt N JJournal of applied microbiology (2009), 107 (2), 368-78 ISSN:.Current models to study Legionella pathogenesis include the use of primary macrophages and monocyte cell lines, various free-living protozoan species and murine models of pneumonia. However, there are very few studies of Legionella spp. pathogenesis aimed at associating the role of biofilm colonization and parasitization of biofilm microbiota and release of virulent bacterial cell/vacuoles in drinking water distribution systems. Moreover, the implications of these environmental niches for drinking water exposure to pathogenic legionellae are poorly understood. This review summarizes the known mechanisms of Legionella spp. proliferation within Acanthamoeba and mammalian cells and advocates the use of the amoeba model to study Legionella pathogenicity because of their close association with Legionella spp. in the aquatic environment. The putative role of biofilms and amoebae in the proliferation, development and dissemination of potentially pathogenic Legionella spp. is also discussed. Elucidating the mechanisms of Legionella pathogenicity development in our drinking water systems will aid in elimination strategies and procedural designs for drinking water systems and in controlling exposure to Legionella spp. and similar pathogens.
52刘汉彦;生物膜和原生动物在军团菌发病机制中的作用：对饮用水的影响。应用微生物学杂志.2009， 107 （2）， 368– 378， DOI： 10.1111/j.1365-2672.2009.04208.x - 53Scheikl, U.; Sommer, R.; Kirschner, A.; Rameder, A.; Schrammel, B.; Zweimuller, I.; Wesner, W.; Hinker, M.; Walochnik, J. Free-living amoebae (FLA) co-occurring with legionellae in industrial waters. Eur. J. Protistol.IF 2.9SCIEJCI 0.69Q3生物学2区2014, 50 (4), 422– 429, DOI: 10.1016/j.ejop.2014.04.002 Google Scholar Google 学术搜索53https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A280%3ADC%252BC2cblvVyhsg%253D%253D&md5=0e75f9aa592e6ae6af5a17256640cd42Free-living amoebae (FLA) co-occurring with legionellae in industrial watersScheikl Ute; Sommer Regina; Kirschner Alexander; Rameder Alexandra; Schrammel Barbara; Zweimuller Irene; Wesner Wolfgang; Hinker Manfred; Walochnik JuliaEuropean journal of protistology (2014), 50 (4), 422-9 ISSN:.Legionella pneumophila is known as the causative agent of Legionnaires' disease and free-living amoebae (FLA) can serve as vehicles for legionellae. The aim of this study was to screen industrial waters for the occurrence of FLA and their co-occurrence with legionellae. A total of 201 water samples, including 129 cooling waters and 72 process waters, and 30 cooling lubricants were included in the study. Treated waters were screened periodically, pre and post treatment. Altogether, 72.6% of the water samples were positive for FLA, acanthamoebae being most prevalent (in 23.9% of the samples) followed by Vermamoeba vermiformis (19.4%). Only one cooling lubricant was positive (Acanthamoeba genotype T4). Legionella spp. were detected in 34.8% of the water samples and in 15% in high concentrations (>1000 CFU/100 ml). Altogether, 81.4% of the Legionella-positive samples were positive for FLA by standard methods. By applying a highly sensitive nested PCR to a representative set of random samples it was revealed that Legionella spp. always co-occurred with Acanthamoeba spp. Although the addition of disinfectants did influence amoebal density and diversity, treated waters showed no difference concerning FLA in the interphases of disinfection. It appears that FLA can re-colonize treated waters within a short period of time.
53Scheikl，美国;索默，R.;基什纳，A.;拉梅德，A.;施拉梅尔，B.;茨魏穆勒，I.;韦斯纳，W.;欣克，M.;Walochnik， J.自由生活的变形虫 （FLA） 与工业水域中的军团菌共生。Eur. J. Protistol.2014， 50 （4）， 422– 429， DOI： 10.1016/j.ejop.2014.04.002 - 54Caicedo, C.; Rosenwinkel, K.-H.; Exner, M.; Verstraete, W.; Suchenwirth, R.; Hartemann, P.; Nogueira, R. Legionella occurrence in municipal and industrial wastewater treatment plants and risks of reclaimed wastewater reuse: Review. Water Res.IF 12.8SCIEJCI 2.15Q1环境科学与生态学1区Top2019, 149, 21– 34, DOI: 10.1016/j.watres.2018.10.080 Google Scholar Google 学术搜索54https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC1cXitFyhurbF&md5=7fbe53b1bb2a7053e7504a0499f2ccabLegionella occurrence in municipal and industrial wastewater treatment plants and risks of reclaimed wastewater reuse: ReviewCaicedo, C.; Rosenwinkel, K.-H.; Exner, M.; Verstraete, W.; Suchenwirth, R.; Hartemann, P.; Nogueira, R.Water Research (2019), 149 (), 21-34CODEN: WATRAG; ISSN:0043-1354. (Elsevier Ltd.)Wastewater treatment plants (WWTPs) have been identified as confirmed but until today underestimated sources of Legionella, playing an important role in local and community cases and outbreaks of Legionnaires' disease. In general, aerobic biol. systems provide an optimum environment for the growth of Legionella due to high org. nitrogen and oxygen concns., ideal temps. and the presence of protozoa. However, few studies have investigated the occurrence of Legionella in WWTPs, and many questions in regards to the interacting factors that promote the proliferation and persistence of Legionella in these treatment systems are still unanswered. This crit. review summarizes the current knowledge about Legionella in municipal and industrial WWTPs, the conditions that might support their growth, as well as control strategies that have been applied. Furthermore, an overview of current quantification methods, guidelines and health risks assocd. with Legionella in reclaimed wastewater is also discussed in depth. A better understanding of the conditions promoting the occurrence of Legionella in WWTPs will contribute to the development of improved wastewater treatment technologies and/or innovative mitigation approaches to minimize future Legionella outbreaks.
54凯塞多，C.;罗森温克尔，K.-H.;埃克斯纳，M.;韦斯特雷特，W.;Suchenwirth，R.;哈特曼，P.;Nogueira， R.军团菌在市政和工业废水处理厂中的发生以及回收废水再利用的风险：综述。水研究2019， 149， 21– 34， DOI： 10.1016/j.watres.2018.10.080 - 55Gerrity, D.; Arnold, M.; Dickenson, E.; Moser, D.; Sackett, J. D.; Wert, E. C. Microbial community characterization of ozone-biofiltration systems in drinking water and potable reuse applications. Water Res.IF 12.8SCIEJCI 2.15Q1环境科学与生态学1区Top2018, 135, 207– 219, DOI: 10.1016/j.watres.2018.02.023 Google Scholar Google 学术搜索There is no corresponding record for this reference.
55杰里蒂，D.;阿诺德，M.;狄更生，E.;莫泽，D.;萨克特，法学博士;Wert， E. C.饮用水和饮用水再利用应用中臭氧生物过滤系统的微生物群落表征。水研究 2018， 135， 207– 219， DOI： 10.1016/j.watres.2018.02.023 - 56Zhang, L.; Graham, N.; Li, G.; Yu, W. Divergent accumulation of membrane biofouling by slight elevation of nitrogen and phosphorus in drinking water treatment: Performances and mechanisms. Water Res.IF 12.8SCIEJCI 2.15Q1环境科学与生态学1区Top2022, 222, 118898, DOI: 10.1016/j.watres.2022.118898 Google Scholar Google 学术搜索There is no corresponding record for this reference.
56张，L.;格雷厄姆，N.;李，G.;Yu， W.饮用水处理中氮磷略微升高的膜生物污垢发散积累：性能和机制。水研究 2022， 222， 118898， DOI： 10.1016/j.watres.2022.118898 - 57Desmond, P.; Huisman, K. T.; Sanawar, H.; Farhat, N. M.; Traber, J.; Fridjonsson, E. O.; Johns, M. L.; Flemming, H.-C.; Picioreanu, C.; Vrouwenvelder, J. S. Controlling the hydraulic resistance of membrane biofilms by engineering biofilm physical structure. Water Res.IF 12.8SCIEJCI 2.15Q1环境科学与生态学1区Top2022, 210, 118031, DOI: 10.1016/j.watres.2021.118031 Google Scholar Google 学术搜索57https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BB38XksFKitQ%253D%253D&md5=ee3251a57598a194d198d95270b37ae8Controlling the hydraulic resistance of membrane biofilms by engineering biofilm physical structureDesmond, Peter; Huisman, Kees Theo; Sanawar, Huma; Farhat, Nadia M.; Traber, Jacqueline; Fridjonsson, Einar O.; Johns, Michael L.; Flemming, Hans-Curt; Picioreanu, Cristian; Vrouwenvelder, Johannes S.Water Research (2022), 210 (), 118031CODEN: WATRAG; ISSN:0043-1354. (Elsevier Ltd.)A review. The application of membrane technol. for water treatment and reuse is hampered by the development of a microbial biofilm. Biofilm growth in micro-and ultrafiltration (MF/UF) membrane modules, on both the membrane surface and feed spacer, can form a secondary membrane and exert resistance to permeation and crossflow, increasing energy demand and decreasing permeate quantity and quality. In recent years, exhaustive efforts were made to understand the chem., structural and hydraulic characteristics of membrane biofilms. In this , we critically assess which specific structural features of membrane biofilms exert resistance to forced water passage in MF/UF membranes systems applied to water and wastewater treatment, and how biofilm phys. structure can be engineered by process operation to impose less hydraulic resistance ("below-the-pain threshold"). Counter-intuitively, biofilms with greater thickness do not always cause a higher hydraulic resistance than thinner biofilms. Dense biofilms, however, had consistently higher hydraulic resistances compared to less dense biofilms. The mechanism by which d. exerts hydraulic resistance is reported in the literature to be dependant on the biofilms' internal packing structure and EPS chem. compd. (e.g., porosity, polymer concn.). Current reports of internal porosity in membrane biofilms are not supported by adequate exptl. evidence or by a reliable methodol., limiting a unified understanding of biofilm internal structure. Identifying the dependency of hydraulic resistance on biofilm d. invites efforts to control the hydraulic resistance of membrane biofilms by engineering internal biofilm structure. Regulation of biofilm internal structure is possible by alteration of key determinants such as feed water nutrient compd./concn., hydraulic shear stress and resistance and can engineer biofilm structural development to decrease d. and therein hydraulic resistance. Future efforts should seek to det. the extent to which the concept of "biofilm engineering" can be extended to other biofilm parameters such as mech. stability and the implication for biofilm control/removal in engineered water systems (e.g., pipelines and/or, cooling towers) susceptible to biofouling.
57德斯蒙德，P.;豪氏威马，K.T.;萨纳瓦尔，H.;新墨西哥州法哈特;特拉伯，J.;弗里琼森，EO;约翰斯，ML;弗莱明，HC;皮西奥雷阿努，C.;Vrouwenvelder， J. S.通过工程生物膜物理结构控制膜生物膜的水力阻力。水研究 2022， 210， 118031， DOI： 10.1016/j.watres.2021.118031 - 58Abada, B.; Safarik, J.; Ishida, K. P.; Chellam, S. Surface characterization of end-of-life reverse osmosis membranes from a full-scale advanced water reuse facility: Combined role of bioorganic materials and silicon on chemically irreversible fouling. J. Membr. Sci.IF 9.5SCIEJCI 1.85Q1工程技术1区Top2022, 653, 120511, DOI: 10.1016/j.memsci.2022.120511 Google Scholar Google 学术搜索58https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BB38XpsVygtLg%253D&md5=451543b823a01355c995ea63b3ba2462Surface characterization of end-of-life reverse osmosis membranes from a full-scale advanced water reuse facility: Combined role of bioorganic materials and silicon on chemically irreversible foulingAbada, Bilal; Safarik, Jana; Ishida, Kenneth P.; Chellam, ShankararamanJournal of Membrane Science (2022), 653 (), 120511CODEN: JMESDO; ISSN:0376-7388. (Elsevier B.V.)Eight-year-old end-of-life reverse osmosis (RO) membranes from all three stages of a full-scale plant from the world's largest potable reuse facility were comprehensively characterized to discern the role of the co-existing foulants on performance decline and recovery by chem. cleaning. XPS and energy dispersive X-ray spectra detected surficial silica foulants on all stages. High-resoln. XPS and IR spectra evidenced siloxanes among other forms of silicon foulants, which was confirmed by gas chromatog.-mass spectrometry as cyclosiloxanes. Addnl., culturable bacteria were recovered, and other bioorg. foulants were identified by colorimetry, microscopy, and spectroscopy. Higher amts. of bioorg. foulants were measured in the first two stages, whereas silica fouling was more significant in the first- and third-stage elements. Chem. cleaning with either sodium tripolyphosphate - sodium dodecylbenzenesulfonic acid mixt., sodium dodecyl sulfate - sodium hydroxide mixt., or hydrochloric acid did not completely restore membrane permeability demonstrating the need for membrane replacement. Siliceous foulants were most intractable to all chem. cleaning methods evaluated (including sodium hydroxide) and were the dominant cause of chem.-irreversible fouling leading to the membranes' end-of-life. Our results suggest that incorporating silicon pretreatment could improve RO performance and extend membrane life span during municipal potable reuse.
58阿巴达，B.;萨法里克，J.;石田，K.P.;Chellam， S.来自全尺寸先进水回用设施的报废反渗透膜的表面表征：生物有机材料和硅对化学不可逆污染的综合作用。J.门布尔。Sci.2022， 653， 120511， DOI： 10.1016/j.memsci.2022.120511 - 59Ivleva, N. P.; Wagner, M.; Horn, H.; Niessner, R.; Haisch, C. Towards a nondestructive chemical characterization of biofilm matrix by Raman microscopy. Anal. Bioanal. Chem.IF 4.3SCIEJCI 0.93Q1化学2区2009, 393 (1), 197– 206, DOI: 10.1007/s00216-008-2470-5 Google Scholar Google 学术搜索There is no corresponding record for this reference.
59伊夫列瓦，N.P.;瓦格纳，M.;霍恩，H.;尼斯纳，R.;Haisch， C.通过拉曼显微镜对生物膜基质进行无损化学表征。肛门。 生物肛门。Chem.2009， 393 （1）， 197– 206， DOI： 10.1007/s00216-008-2470-5 - 60Laue, H.; Schenk, A.; Li, H.; Lambertsen, L.; Neu, T. R.; Molin, S.; Ullrich, M. S. Contribution of alginate and levan production to biofilm formation by Pseudomonas syringae. Microbiolology 2006, 152 (10), 2909– 2918, DOI: 10.1099/mic.0.28875-0 Google Scholar Google 学术搜索There is no corresponding record for this reference.
60劳厄，H.;申克，A.;李旭;兰伯特森，L.;诺伊，TR;莫林，S.;Ullrich， M. S.丁香假单胞菌对海藻酸盐和莱万生产对生物膜形成的贡献。微生物学 2006， 152 （10）， 2909– 2918， DOI： 10.1099/mic.0.28875-0
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Abstract 抽象
Figure 1 图1
Figure 1. Molecular-level DOM compositional patterns of the influents. (A) Regions of the van Krevelen diagram based on ratios of O/C and H/C. (B–D) Van Krevelen diagrams of influent DOM in the control, ratio 0.5, and ratio 1 membrane filtration systems, respectively. (E) Regional proportion of the DOM molecules. (F) Venn diagram of the molecular DOM formulas shared in the different samples. (G) Proportion of CHO, CHON, CHOS, and CHONS molecules in control, ratio 0.5, and ratio 1 influents. (H,I) Distribution of AI and NOSC values for molecular formulas of the influent DOM, respectively. Significant differences were investigated using the Kruskal–Wallis test. The marks a, b, and c in bold indicate statistical significance at P < 0.05.
图 1.进水物的分子水平DOM组成模式。（A） 基于 O/C 和 H/C 比率的 van Krevelen 图的区域。 （b–D） 分别是控制、比率 0.5 和比率 1 膜过滤系统中进水 DOM 的 Van Krevelen 图。（E） DOM分子的区域比例。（F） 不同样品中共享的分子DOM分子式的维恩图。（G） 对照组 CHO、CHON、CHOS 和 CHONS 分子的比例，比例为 0.5，比例为 1。（H，I）进水DOM分子式AI和NOSC值的分布。使用 Kruskal-Wallis 检验研究了显着差异。粗体标记 a、b 和 c 表示 P < 0.05 时的统计学显著性。Figure 2 图2
Figure 2. Compositional and diversity patterns of biofilm microbial consortium. (A) Upset plot of the average number of bacterial ASVs shared in the control, ratio 0.5, and ratio 1 biofilms. (B,C) Average relative abundance of bacterial taxa at phylum and genus levels, respectively. (D–G) Shannon, Simpson, Chao 1, and Pielou evenness indexes of the biofilm microbial consortium, respectively. (H) PCoA plot of the biofilm bacterial communities based on the Bray–Curtis distance matrix. (I) Bray–Curtis dissimilarity of bacterial community across different biofilms. Significant differences were investigated using the Kruskal–Wallis test. The marks a, b, and c in bold indicate statistical significance at P < 0.05.
图2.生物膜微生物联盟的组成和多样性模式。（A） 对照中共享的细菌 ASV 平均数量的扰动图，比率 0.5 和比率 1 生物膜。（乙、丙）细菌类群在门和属水平上的平均相对丰度。（D-G）Shannon、Simpson、Chao 1 和 Pielou 分别是生物膜微生物联盟的均匀度指数。（H） 基于Bray-Curtis距离矩阵的生物膜细菌群落PCoA图。（I）不同生物膜上细菌群落的Bray-Curtis差异。使用 Kruskal-Wallis 检验研究了显着差异。粗体标记 a、b 和 c 表示 P < 0.05 时的统计学显著性。Figure 3 图3
Figure 3. Morphological and chemical structure of biofilms. (A,B) SEM images of biofilms captured in cross-section and top surface, respectively. (C,D) XPS spectra of the biofilms based on elements C and O, respectively.
图3.生物膜的形态和化学结构。（甲、乙）分别在横截面和顶面捕获的生物膜的SEM图像。（C，D）分别基于元素 C 和 O 的生物膜的 XPS 光谱。Figure 4 图4
Figure 4. Physicochemical properties of the biofilm matrix. (A) Representative fluorescence spectra of the DOM extracted in the biofilm matrix with phosphate buffer solution. (B) Representative FTIR spectra. (C) Representative optical micrographs and the corresponding surface roughness. (D) Concentrations of polysaccharides and proteins. (E) Representative Raman spectra. Significant differences were assessed by the Kruskal–Wallis test and * represents P < 0.05.
图4.生物膜基质的物理化学性质。（A）用磷酸盐缓冲溶液在生物膜基质中提取的DOM的代表性荧光光谱。（B） 具有代表性的傅里叶变换红外光谱。（C）具有代表性的光学显微照片和相应的表面粗糙度。（D） 多糖和蛋白质的浓度。（E） 具有代表性的拉曼光谱。通过 Kruskal-Wallis 检验评估显著差异，* 表示 P < 0.05。Figure 5 图5
Figure 5. Filtration performance of membrane systems. (A) Representative fluorescence spectra of DOM in the influents and effluents of membrane filtration systems. (B) Regional removal rate of fluorescence intensity by the membrane filtration systems. (C) Apparent molecular weight distribution profile of the DOM in the influents and effluents. (D) Hydraulic resistance of the membrane system in the course of filtration.
图5.膜系统的过滤性能。（A）DOM在膜过滤系统进水和出水中的代表性荧光光谱。（B）膜过滤系统对荧光强度的区域去除率。（C） DOM在进水和出水中的表观分子量分布曲线。（D）过滤过程中膜系统的水力阻力。References
ARTICLE SECTIONSThis article references 60 other publications.
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- 3Yu, W.; Xu, L.; Graham, N.; Qu, J. Pre-treatment for ultrafiltration: Effect of pre-chlorination on membrane fouling. Sci. Rep.IF 4.6SCIEJCI 1.06Q2综合性期刊2区2014, 4, 6513, DOI: 10.1038/srep06513 3https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC2MXksVWmsbo%253D&md5=315394adaa8ecb9b3fd01f3f45d8263aPre-treatment for ultrafiltration: effect of pre-chlorination on membrane foulingYu, Wenzheng; Xu, Lei; Graham, Nigel; Qu, JiuhuiScientific Reports (2014), 4 (), 6513CODEN: SRCEC3; ISSN:2045-2322. (Nature Publishing Group)Microbial effects are believed to be a major contributor to membrane fouling in drinking water treatment. Sodium hypochlorite (NaClO) is commonly applied in membrane cleaning, but its potential use as a pretreatment for controlling operational fouling has received little attention. In this study, the effect of adding a continuous low dose of NaClO (1 mg/l as active Cl) in combination with alum, before ultrafiltration, was compared with only alum as pretreatment. The results showed that the addn. of NaClO substantially reduced membrane fouling both in terms of the rate of TMP development and the properties of the membrane cake layer. Although the size of nano-scale primary coagulant flocs changed little by the addn. of NaClO, the cake layer on the membrane had a greater porosity and a substantially reduced thickness. NaClO was found to inactivate bacteria in the influent flow, which reduced both microbial proliferation and the prodn. of proteins and polysaccharides in the cake layer and contributed significantly to improving the overall ultrafiltration performance. NaClO dosing had no adverse impact on the formation of currently regulated disinfection byproduct compds. (THMs and HAAs).
- 4Liu, T.; Chen, Z.-L.; Yu, W.-Z.; You, S.-J. Characterization of organic membrane foulants in a submerged membrane bioreactor with pre-ozonation using three-dimensional excitation-emission matrix fluorescence spectroscopy. Water Res.IF 12.8SCIEJCI 2.15Q1环境科学与生态学1区Top2011, 45 (5), 2111– 2121, DOI: 10.1016/j.watres.2010.12.023 4https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC3MXitFaqurY%253D&md5=d8862c5f758d9b4d58f6d80045804e9dCharacterization of organic membrane foulants in a submerged membrane bioreactor with pre-ozonation using three-dimensional excitation-emission matrix fluorescence spectroscopyLiu, Ting; Chen, Zhong-lin; Yu, Wen-zheng; You, Shi-jieWater Research (2011), 45 (5), 2111-2121CODEN: WATRAG; ISSN:0043-1354. (Elsevier B.V.)This study focuses on org. membrane foulants in a submerged membrane bioreactor (MBR) process with pre-ozonation compared to an individual MBR using three-dimensional excitation-emission matrix (EEM) fluorescence spectroscopy. While the influent was continuously ozonated at a normal dosage, preferable org. matter removal was achieved in subsequent MBR, and trans-membrane pressure increased at a much lower rate than that of the individual MBR. EEM fluorescence spectroscopy was employed to characterize the dissolved org. matter (DOM) samples, extracellular polymeric substance (EPS) samples and membrane foulants. Four main peaks could be identified from the EEM fluorescence spectra of the DOM samples in both MBRs. Two peaks were assocd. with the protein-like fluorophores, and the other ones were related to the humic-like fluorophores. The results indicated that pre-ozonation decreased fluorescence intensities of all peaks in the EEM spectra of influent DOM esp. for protein-like substances and caused red shifts of all fluorescence peaks to different extents. The peak intensities of the protein-like substances represented by Peak T1 and T2 in EPS spectra were obviously decreased as a result of pre-ozonation. Both external and internal fouling could be effectively mitigated by the pre-ozonation. The most primary component of external foulants was humic acid-like substance (Peak C) in the MBR with pre-ozonation and protein-like substance (Peak T1) in the individual MBR, resp. The content decrease of protein-like substances and structural change of humic-like substances were obsd. in external foulants from EEM fluorescence spectra due to pre-ozonation. However, it could be seen that ozonation resulted in significant redn. of intensities but little location shift of all peaks in EEM fluorescence spectra of internal foulants.
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- 6Hammes, F.; Berney, M.; Wang, Y.; Vital, M.; Koster, O.; Egli, T. Flow-cytometric total bacterial cell counts as a descriptive microbiological parameter for drinking water treatment processes. Water Res.IF 12.8SCIEJCI 2.15Q1环境科学与生态学1区Top2008, 42 (1–2), 269– 277, DOI: 10.1016/j.watres.2007.07.009 6https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BD2sXhsVGlur%252FF&md5=6ab3931f0b41fa3150749dd4f76f71c9Flow-cytometric total bacterial cell counts as a descriptive microbiological parameter for drinking water treatment processesHammes, Frederik; Berney, Michael; Wang, Yingying; Vital, Marius; Koester, Oliver; Egli, ThomasWater Research (2008), 42 (1-2), 269-277CODEN: WATRAG; ISSN:0043-1354. (Elsevier Ltd.)There are significantly more microbial cells in drinking water than what can be cultured on synthetic growth media. Nonetheless, cultivation-based heterotrophic plate counts (HPCs) are used worldwide as a general microbial quality parameter in drinking water treatment and distribution. Total bacterial cell concns. are normally not considered during drinking water treatment as a design, operative or legislative parameters. This is mainly because easy and rapid methods for quantification of total bacterial cell concns. have, up to now, not been available. As a consequence, the existing lack of data does not allow demonstrating the practical value of this parameter. We used fluorescence staining of microbial cells with the nucleic acid stain SYBR Green I together with quant. flow cytometry (FCM) to analyze total cell concns. in water samples from a drinking water pilot plant. The plant treats surface water (Lake Zuerich) through sequential ozonization, granular activated C (GAC) filtration and membrane ultrafiltration (UF). The data were compared with adenosine tri-phosphate (ATP) measurements and conventional HPCs performed on the same water samples. We demonstrated that the impact of all 3 major treatment steps on the microbiol. in the system could accurately be described with total cell counting: ozonization caused chem. destruction of the bacterial cells; GAC filtration facilitated significant regrowth of the microbial community; and membrane UF phys. removed the bacterial cells from the water. FCM typically detected 1-2 log units more than HPC, while ATP measurements were prone to interference from extracellular ATP released during the ozonation step in the treatment train. We show that total cell concn. measured with FCM is a rapid, easy, sensitive and importantly, a descriptive parameter of several widely applied drinking water treatment processes.
- 7Jiang, T.; Tian, T.; Guan, Y.-F.; Yu, H.-Q. Contrasting behaviors of pre-ozonation on ceramic membrane biofouling: Early stage vs late stage. Water Res.IF 12.8SCIEJCI 2.15Q1环境科学与生态学1区Top2022, 220, 118702, DOI: 10.1016/j.watres.2022.118702 7https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BB38XhsFGhurnJ&md5=ac3d150b83c4b2f3f122c42c69945e17Contrasting behaviors of pre-ozonation on ceramic membrane biofouling: Early stage vs late stageJiang, Ting; Tian, Tian; Guan, Yan-Fang; Yu, Han-QingWater Research (2022), 220 (), 118702CODEN: WATRAG; ISSN:0043-1354. (Elsevier Ltd.)Pre-ozonation coupled with ceramic membrane filtration has been widely used to alleviate membrane fouling. However, information on the efficiency and underlying mechanism of pre-ozonation in the evolution of ceramic membrane biofouling is limited. Herein, filtration expts. with a synthesis wastewater contg. activated sludge were conducted in a cross-flow system to evaluate the effects of pre-ozonation on ceramic membrane biofouling. Result of flux tests show that pre-ozonation aggravated biofouling at the early stage, but alleviated the biofouling at the late stage. In situ FTIR spectra show that the aggravated biofouling with pre-ozonation was mainly caused by the enhanced complexation between phosphate group from DNA and Al2O3 surface and the increased rigid of proteins' structure. At the early stage, more severe pore blockage further substantiated the higher permeate resistance. By contrast, more dead cells were obsd. on membrane surface at the late stage, indicating the prevention of biofouling development after long-term pre-ozonation. Addnl., the structures and compns. of cake layers at the early and late stages exhibited considerable differences accompanied by the variation in microbial community with the evolution of biofouling. Therefore, this work demonstrates the effectiveness of pre-ozonation in biofouling in long-term operation and provides mechanistic insights into the evolution of biofouling on ceramic membrane.
- 8Du, J. Y.; Wang, C.; Zhao, Z. W.; Chen, R.; Zhang, P. F.; Cui, F. Y. Effect of vacuum ultraviolet/ozone pretreatment on alleviation of ultrafiltration membrane fouling caused by algal extracellular and intracellular organic matter. ChemosphereIF 8.8SCIEJCI 1.55Q1环境科学与生态学2区Top2022, 305, 135455, DOI: 10.1016/j.chemosphere.2022.135455 8https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BB38XhsF2qsrnP&md5=26ba12e172eb505a881aae8f611b9b35Effect of vacuum ultraviolet/ozone pretreatment on alleviation of ultrafiltration membrane fouling caused by algal extracellular and intracellular organic matterDu, Jinying; Wang, Chuang; Zhao, Zhiwei; Chen, Rui; Zhang, Pengfei; Cui, FuyiChemosphere (2022), 305 (), 135455CODEN: CMSHAF; ISSN:0045-6535. (Elsevier Ltd.)Algal blooms in source water can cause algal org. matter (AOM)-related membrane fouling in drinking water treatment. Herein, the effects of vacuum UV/ozone (VUV/O3) pretreatment on alleviating ultrafiltration membrane fouling caused by AOM, including extracellular org. matter (EOM) and intracellular org. matter (IOM), were investigated systematically. Compared to its sub-processes (UV/O3, O3, VUV, and UV), VUV/O3 pretreatment showed the best performance on AOM removal and membrane fouling mitigation. After VUV/O3 pretreatment, the DOC of EOM and IOM in feed decreased by 51.1% and 26.7%, resp., and fluorescence components and UV254 of EOM and IOM in feed decreased obviously. Hence, the final specific fluxes of the membranes increased significantly under the impacts of VUV/O3, and VUV/O3 achieved 89.5% and 97.2% mitigation of reversible fouling caused by EOM and IOM, resp. VUV/O3 pretreatment also reduced the foulants on membrane surface and surface roughness. Moreover, under the effects of reactive oxygen species oxidn., VUV photolysis, and direct O3 oxidn., VUV/O3 decreased org. load and changed the mol. wt. distribution, hydrophilicity, and interaction-free energy of AOM, thus mitigating membrane fouling. Furthermore, the effects of O3 dosage and mol. wt. cut-off of ultrafiltration membrane on membrane fouling mitigation by VUV/O3 were also investigated. All results highlighted that VUV/O3 pretreatment had huge potential in mitigating AOM-induced membrane fouling.
- 9Yu, W.; Liu, T.; Crawshaw, J.; Liu, T.; Graham, N. Ultrafiltration and nanofiltration membrane fouling by natural organic matter: Mechanisms and mitigation by pre-ozonation and pH. Water Res.IF 12.8SCIEJCI 2.15Q1环境科学与生态学1区Top2018, 139, 353– 362, DOI: 10.1016/j.watres.2018.04.025 9https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC1cXns1WmsLs%253D&md5=420aabcd3a3d86d667c671cfbf6ea2f5Ultrafiltration and nanofiltration membrane fouling by natural organic matter: Mechanisms and mitigation by pre-ozonation and pHYu, Wenzheng; Liu, Teng; Crawshaw, John; Liu, Ting; Graham, NigelWater Research (2018), 139 (), 353-362CODEN: WATRAG; ISSN:0043-1354. (Elsevier Ltd.)The fouling of ultrafiltration (UF) and nanofiltration (NF) membranes during the treatment of surface waters continues to be of concern and the particular role of natural org. matter (NOM) requires further investigation. In this study the effect of pH and surface charge on membrane fouling during the treatment of samples of a representative surface water (Hyde Park recreational lake) were evaluated, together with the impact of pre-ozonation. While biopolymers in the surface water could be removed by the UF membrane, smaller mol. wt. (MW) fractions of NOM were poorly removed, confirming the importance of membrane pore size. For NF membranes the removal of smaller MW fractions (800Da-10kDa) was less than expected from their pore size; however, nearly all of the hydrophobic, humic-type substances could be removed by the hydrophilic NF membranes for all MW distributions (greater than 90%). The results indicated the importance of the charge and hydrophilic nature of the NOM. Thus, the hydrophilic NF membrane could remove the hydrophobic org. matter, but not the hydrophilic substances. Increasing charge effects (more neg. zeta potentials) with increasing soln. pH were found to enhance orgs. removal and reduce fouling (flux decline), most likely through greater membrane surface repulsion. Pre-ozonation of the surface water increased the hydrophilic fraction and anionic charge of NOM and altered their size distributions. This resulted in a decreased fouling (less flux decline) for the UF and smaller pore NF, but a slight increase in fouling for the larger pore NF. The differences in the NF behavior are believed to relate to the relative sizes of ozonated org. fractions and the NF pores; a similar size of ozonated org. fractions and the NF pores causes significant membrane fouling.
- 10Wang, L.; Song, S.; Xu, L.; Graham, N. J. D.; Yu, W. Z. Beneficial role of pre- and post-ozonation in a low rate biofiltration-ultrafiltration process treating reclaimed water. Water Res.IF 12.8SCIEJCI 2.15Q1环境科学与生态学1区Top2022, 226, 119284, DOI: 10.1016/j.watres.2022.119284 There is no corresponding record for this reference.
- 11Jennings, E.; Kremser, A.; Han, L. M.; Reemtsma, T.; Lechtenfeld, O. J. Discovery of polar ozonation byproducts via direct injection of effluent organic matter with online LC-FT-ICR-MS. Environ. Sci. Technol.IF 11.4SCIEJCI 1.44Q1环境科学与生态学1区Top2022, 56 (3), 1894– 1904, DOI: 10.1021/acs.est.1c04310 11https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BB38XlvVCjtg%253D%253D&md5=612f9cbdc1d13d9f3af1c3c92ebc33c8Discovery of polar ozonation byproducts via direct injection of effluent organic matter with online LC-FT-ICR-MSJennings, Elaine; Kremser, Arina; Han, Limei; Reemtsma, Thorsten; Lechtenfeld, Oliver J.Environmental Science & Technology (2022), 56 (3), 1894-1904CODEN: ESTHAG; ISSN:1520-5851. (American Chemical Society)Effluent org. matter (EfOM), a major ozone consumer during wastewater ozonation, is a complex mixt. of natural and anthropogenic org. mols. Ozonation of EfOM adds to mol. complexity by introducing polar and potentially mobile ozonation byproducts (OBPs). Currently, nontargeted direct infusion (DI) ultrahigh resoln. mass spectrometry (e.g. FT-ICR-MS) is used to study OBPs but requires sample extn., limiting the accessible polarity range of OBPs. To better understand the impact of ozonation on EfOM and the formation of polar OBPs, nonextd. effluent was analyzed by direct injection onto a reversed-phase liq. chromatog. system (RP-LC) online hyphenated with an FT-ICR-MS. Over four times more OBPs were detected in nonextd. EfOM compared to effluent extd. with solid phase extn. and measured with DI-FT-ICR-MS (13817 vs 3075). Over 1500 highly oxygenated OBPs were detected exclusively in early eluting fractions of nonextd. EfOM, indicating polar OBPs. Oxygenation of these newly discovered OBPs is higher than previously found, with an av. mol. DBE-O value of -3.3 and O/C ratio of 0.84 in the earliest eluting OBP fractions. These polar OBPs are consistently lost during extn. but may play an important role in understanding the environmental impact of ozonated EfOM. Moreover, 316 mol. formulas classified as nonreactive to ozone in DI-FT-ICR-MS can be identified with LC-FT-ICR-MS as isomers with varying degrees of reactivity, providing for the first time exptl. evidence of differential reactivity of complex org. matter isomers with ozone.
- 12Phungsai, P.; Kurisu, F.; Kasuga, I.; Furumai, H. Changes in dissolved organic matter composition and disinfection byproduct precursors in advanced drinking water treatment processes. Environ. Sci. Technol.IF 11.4SCIEJCI 1.44Q1环境科学与生态学1区Top2018, 52 (6), 3392– 3401, DOI: 10.1021/acs.est.7b04765 12https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC1cXjtVemurk%253D&md5=7f763252275b4c420cda1a79feab6d19Changes in Dissolved Organic Matter Composition and Disinfection Byproduct Precursors in Advanced Drinking Water Treatment ProcessesPhungsai, Phanwatt; Kurisu, Futoshi; Kasuga, Ikuro; Furumai, HiroakiEnvironmental Science & Technology (2018), 52 (6), 3392-3401CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)Mol. changes in dissolved org. matter (DOM) from treatment processes at two drinking water treatment plants in Japan were investigated using unknown screening anal. by Orbitrap mass spectrometry. DOM formulas with carbon, hydrogen and oxygen (CHO-DOM) were the most abundant class in water samples, and over half of them were commonly found at both plants. Among the treatment processes, ozonization induced the most drastic changes to DOM. Mass peak intensities of less satd. CHO-DOM (pos. (oxygen subtracted double bond equiv. per carbon (DBE-O)/C)) decreased by ozonization, while more satd. oxidn. byproducts (neg. (DBE-O)/C) increased and new oxidn. byproducts (OBPs) were detected. By Kendrick mass anal., ozone reactions preferred less satd. CHO-DOM in the same alkylation families and produced more satd. alkylation families of OBPs. Following ozonization, biol. activated carbon filtration effectively removed <300 Da CHO-DOM, including OBPs. Following chlorination, over 50 chlorinated formulas of disinfection byproducts (DBPs) were found in chlorinated water samples where at least half were unknown. Putative precursors of these DBPs were detd. based on electrophilic substitutions and addn. reactions. Ozonization demonstrated better decompn. of addn. reaction-type precursors than electrophilic substitution-type precursors; over half of both precursor types decreased during biol. activated carbon filtration.
- 13von Gunten, U. Ozonation of drinking water: Part I. Oxidation kinetics and product formation. Water Res.IF 12.8SCIEJCI 2.15Q1环境科学与生态学1区Top2003, 37 (7), 1443– 1467, DOI: 10.1016/S0043-1354(02)00457-8 13https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BD3sXhtlGqsr4%253D&md5=a71315929c55e466b0f0f0a8908eebb3Ozonation of drinking water: Part I. Oxidation kinetics and product formationvon Gunten, UrsWater Research (2003), 37 (7), 1443-1467CODEN: WATRAG; ISSN:0043-1354. (Elsevier Science Ltd.)A review is given. The oxidn. of org. and inorg. compds. during ozonization can occur via ozone or OH radicals or a combination thereof. The oxidn. pathway is detd. by the ratio of ozone and OH radical concns. and the corresponding kinetics. A huge database with several hundred rate consts. for ozone and a few thousand rate consts. for OH radicals is available. Ozone is an electrophile with a high selectivity. The 2nd-order rate consts. for oxidn. by ozone vary over 10 orders of magnitude, <0.1-7 × 109/M-s. The reactions of ozone with drinking-water relevant inorg. compds. are typically fast and occur by an oxygen atom transfer reaction. Org. micropollutants are oxidized with ozone selectively. Ozone reacts mainly with double bonds, activated arom. systems and non-protonated amines. In general, electron-donating groups enhance the oxidn. by ozone whereas electron-withdrawing groups reduce the reaction rates. The kinetics of direct ozone reactions depend strongly on the speciation (acid-base, metal complexation). The reaction of OH radicals with the majority of inorg. and org. compds. is nearly diffusion-controlled. The degree of oxidn. by ozone and OH radicals is given by the corresponding kinetics. Product formation from the ozonation of org. micropollutants in aq. systems has only been established for a few compds.
- 14von Gunten, U. Ozonation of drinking water: Part II. Disinfection and by-product formation in presence of bromide, iodide or chlorine. Water Res.IF 12.8SCIEJCI 2.15Q1环境科学与生态学1区Top2003, 37 (7), 1469– 1487, DOI: 10.1016/S0043-1354(02)00458-X 14https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BD3sXhtlGqsr8%253D&md5=ba68eddfcd8c59a62e16885393b6f0d5Ozonation of drinking water: Part II. Disinfection and by-product formation in presence of bromide, iodide or chlorinevon Gunten, UrsWater Research (2003), 37 (7), 1469-1487CODEN: WATRAG; ISSN:0043-1354. (Elsevier Science Ltd.)A review is given. Proper rate consts. for the inactivation of microorganisms are only available for 6 species (E. coli, Bacillus subtilis spores, Rotavirus, Giardia lamblia cysts, Giardia muris cysts, Cryptosporidium parvum oocysts). The apparent activation energy for the inactivation of bacteria is in the same order as most chem. reactions (35-50 KJ/mol), whereas it is much higher for the inactivation of protozoa (80 KJ/mol). This requires significantly higher ozone exposures at low temps. to get a similar inactivation for protozoa. Even for the inactivation of resistant microorganisms, OH radicals only play a minor role. Numerous org. and inorg. ozonation disinfection/oxidn. byproducts have been identified. The byproduct of main concern is bromate, which is formed in bromide-contg. waters. A low drinking water std. of 10 μg/L has been set for bromate. Therefore, disinfection and oxidn. processes have to be evaluated to fulfil these criteria. In certain cases, when bromide concns. are above about 50 μg/L, it may be necessary to use control measures to lower bromate formation (lowering of pH, ammonia addn.). Iodate is the main byproduct formed during ozonation of iodide-contg. waters. The reactions involved are direct ozone oxidns. Iodate is considered non-problematic because it is transformed back to iodide endogenically. Chloride cannot be oxidized during ozonation processes under drinking water conditions. Chlorate is only formed if a preoxidn. by chlorine and/or chlorine dioxide has occurred.
- 15Wenk, J.; Aeschbacher, M.; Salhi, E.; Canonica, S.; von Gunten, U.; Sander, M. Chemical oxidation of dissolved organic matter by chlorine dioxide, chlorine, and ozone: Effects on its optical and antioxidant properties. Environ. Sci. Technol.IF 11.4SCIEJCI 1.44Q1环境科学与生态学1区Top2013, 47 (19), 11147– 11156, DOI: 10.1021/es402516b 15https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC3sXhtleksbbE&md5=11bda373fa816d65351e83e1b8e3b9f1Chemical Oxidation of Dissolved Organic Matter by Chlorine Dioxide, Chlorine, and Ozone: Effects on Its Optical and Antioxidant PropertiesWenk, Jannis; Aeschbacher, Michael; Salhi, Elisabeth; Canonica, Silvio; von Gunten, Urs; Sander, MichaelEnvironmental Science & Technology (2013), 47 (19), 11147-11156CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)In water treatment dissolved org. matter (DOM) is typically the major sink for chem. oxidants. The resulting changes in DOM, such as its optical properties have been measured to follow the oxidn. processes. However, such measurements contain only limited information on the changes in the oxidn. states of and the reactive moieties in the DOM. We used mediated electrochem. oxidn. to quantify changes in the electron donating capacities (EDCs), and hence the redox states, of 3 different types of DOM during oxidn. with ClO2, Cl (as HOCl/OCl-), and O3. Treatment with ClO2 and HOCl resulted in comparable and prominent decreases in EDCs, while the UV light absorbances of the DOM decreased only slightly. Conversely, ozonization resulted in only small decreases of the EDCs but pronounced absorbance losses of the DOM. These results suggest that ClO2 and HOCl primarily reacted as oxidants by accepting electrons from electron-rich phenolic and hydroquinone moieties in the DOM, while O3 reacted via electrophilic addn. to arom. moieties, followed by ring cleavage. This study highlights the potential of combined EDC-UV measurements to monitor chem. oxidn. of DOM, to assess the nature of the reactive moieties and to study the underlying reaction pathways.
- 16Remucal, C. K.; Salhi, E.; Walpen, N.; von Gunten, U. Molecular-level transformation of dissolved organic matter during oxidation by ozone and hydroxyl radical. Environ. Sci. Technol.IF 11.4SCIEJCI 1.44Q1环境科学与生态学1区Top2020, 54 (16), 10351– 10360, DOI: 10.1021/acs.est.0c03052 16https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BB3cXhsVegt7zE&md5=f98f8139a31c6facb1fd377748fb2c28Molecular-level transformation of dissolved organic matter during oxidation by ozone and hydroxyl radicalRemucal, Christina K.; Salhi, Elisabeth; Walpen, Nicolas; von Gunten, UrsEnvironmental Science & Technology (2020), 54 (16), 10351-10360CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)Ozonation of drinking and wastewater relies on ozone (O3) and hydroxyl radical (•OH) as oxidants. Both oxidants react with dissolved org. matter (DOM) and alter its compn., but the selectivity of the two oxidants and mechanisms of reactivity with DOM moieties are largely unknown. The reactions of O3 and •OH with two DOM isolates were studied by varying specific ozone doses (0.1-1.3 mg-O3/mg-C) at pH 7. Addnl., conditions that favor O3 (i.e., addn. of an •OH scavenger) or •OH (i.e., pH 11) were investigated. Ozonation decreases aromaticity, apparent mol. wt., and electron donating capacity (EDC) of DOM with large changes obsd. when O3 is the main oxidant (e.g., EDC decreases 63-77% for 1.3 mg-O3/mg-C). Both O3 and •OH react with highly arom., reduced formulas detected using high-resoln. mass spectrometry (O:C = 0.48 ± 0.12; H:C = 1.06 ± 0.23), while •OH also oxidizes more satd. formulas (H:C = 1.64 ± 0.26). Established reactions between model compds. and O3 (e.g., addn. of one to two oxygen atoms) or •OH (e.g., addn. of one oxygen atom and decarboxylation) are obsd. and produce highly oxidized DOM (O:C > 1.0). This study provides mol.-level evidence for the selectivity of O3 as an oxidant within DOM.
- 17Camel, V.; Bermond, A. The use of ozone and associated oxidation processes in drinking water treatment. Water Res.IF 12.8SCIEJCI 2.15Q1环境科学与生态学1区Top1998, 32 (11), 3208– 3222, DOI: 10.1016/S0043-1354(98)00130-4 17https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADyaK1cXmslaqtrs%253D&md5=cd3b8501013d0719470cdc43fa41fb5fThe use of ozone and associated oxidation processes in drinking water treatmentCamel, V.; Bermond, A.Water Research (1998), 32 (11), 3208-3222CODEN: WATRAG; ISSN:0043-1354. (Elsevier Science Ltd.)A review, with many refs., summarizes the main applications of ozonization and assocd. oxidn. processes in the treatment of surface water and groundwater for drinking water prodn. Oxidants may be added at several points throughout the treatment: pre-oxidn., intermediate oxidn. or final disinfection. So, the numerous effects of chem. oxidn. are discussed along the water treatment: removal of inorg. species, aid to the coagulation-flocculation process, degrdn. of org. matter and disinfection. Of prime importance in potable water prodn. is the removal of org. matter (natural humic substances, as well as micropollutants, esp. pesticides) to avoid degrdn. of the distributed water (mainly bad odors and tastes; formation of disinfection byproducts such as trihalomethanes; microbial regrowth in the distribution system). Consequently, this point has been particularly detailed. Complete mineralization hardly occurs during the process; as a consequence, further treatment (i.e. sand or granular activated C filtration) is required to improve the distributed water quality, and to meet the drinking water regulations.
- 18Headley, J. V.; Kumar, P.; Dalai, A.; Peru, K. M.; Bailey, J.; McMartin, D. W.; Rowland, S. M.; Rodgers, R. P.; Marshall, A. G. Fourier transform ion cyclotron resonance mass spectrometry characterization of treated Athabasca oil sands processed waters. Energy FuelsIF 5.3SCIEJCI 0.66Q1工程技术3区2015, 29 (5), 2768– 2773, DOI: 10.1021/ef502007b 18https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC2cXhvVygsrjP&md5=a886900067d550434bde1829101028b1Fourier Transform Ion Cyclotron Resonance Mass Spectrometry Characterization of Treated Athabasca Oil Sands Processed WatersHeadley, John V.; Kumar, Pardeep; Dalai, Ajay; Peru, Kerry M.; Bailey, Jon; McMartin, Dena W.; Rowland, Steven M.; Rodgers, Ryan P.; Marshall, Alan G.Energy & Fuels (2015), 29 (5), 2768-2773CODEN: ENFUEM; ISSN:0887-0624. (American Chemical Society)Ultrahigh-resoln. neg.-ion electrospray ionization Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS) was used to characterize Athabasca oil sands processed water (OSPW) treated by (A) coagulation flocculent with lime and bentonite, (B) coagulation flocculent with lime and bentonite followed by activated carbon, and (C) combined ozonation and ultrasonication. Treatment A was ineffective in reducing the level of total naphthenic acid fraction components [NAFCs, defined as the acid-extractable fraction of OSPWs or crude oils (CnH2n + zOwSxNy), where the values n, w, x, and y indicate the no. of carbon, oxygen, sulfur, and nitrogen atoms, resp., and z represents the hydrogen atom deficiency because of the presence of double bonds and ring formation]. Likewise, for treatment A, little or no change was obsd. for the double bond equiv. (DBE) distributions of the compd. classes. Treatments B and C resulted in the redn. of total NAFCs by 26 ± 1.4 and 89 ± 1.1%, resp. For the latter treatments, there was evidence for selective removal of the S and OxSy heteroat. species at the mol. level, along with a redn. in the DBE values for all species.
- 19Scholes, R. C.; King, J. F.; Mitch, W. A.; Sedlak, D. L. Transformation of trace organic contaminants from reverse osmosis concentrate by open-water unit-process wetlands with and without ozone pretreatment. Environ. Sci. Technol.IF 11.4SCIEJCI 1.44Q1环境科学与生态学1区Top2020, 54 (24), 16176– 16185, DOI: 10.1021/acs.est.0c04406 19https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BB3cXisVGhu7bF&md5=306159352fefb5abcfcb2b1a97410294Transformation of trace organic contaminants from reverse osmosis concentrate by open-water unit-process wetlands with and without ozone pretreatmentScholes, Rachel C.; King, Jacob F.; Mitch, William A.; Sedlak, David L.Environmental Science & Technology (2020), 54 (24), 16176-16185CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)Reverse osmosis (RO) treatment of municipal wastewater effluent is becoming more common as water reuse is implemented in water-stressed regions. Where RO conc. is discharged with limited diln., concns. of trace org. contaminants could pose risks to aquatic ecosystems. To provide a low-cost option for removing trace org. compds. from RO conc., a pilot-scale treatment system comprising open-water unit-process wetlands with and without ozone pretreatment was studied over a 2-yr period. A suite of ecotoxicol. relevant org. contaminants was partially removed via photo- and bio-transformations, including β-adrenergic blockers, antivirals, antibiotics, and pesticides. Biotransformation rates were as fast as or up to approx. 50% faster than model predictions based upon data from open-water wetlands that treated municipal wastewater effluent. Phototransformation rates were comparable to or as much as 60% slower than those predicted by models that accounted for light penetration and scavenging of reactive oxygen species. Several compds. were transformed during ozone pretreatment that were poorly removed in the open-water wetland. The combined treatment system resulted in a decrease in the risk quotients of trace org. contaminants in the RO conc., but still diln. may be required to protect sensitive species from urban-use pesticides with low environmental effect concns.
- 20Hubner, U.; von Gunten, U.; Jekel, M. Evaluation of the persistence of transformation products from ozonation of trace organic compounds: A critical review. Water Res.IF 12.8SCIEJCI 2.15Q1环境科学与生态学1区Top2015, 68, 150– 170, DOI: 10.1016/j.watres.2014.09.051 There is no corresponding record for this reference.
- 21Papageorgiou, A.; Voutsa, D.; Papadakis, N. Occurrence and fate of ozonation by-products at a full-scale drinking water treatment plant. Sci. Total Environ.IF 9.8SCIEJCI 1.68Q1环境科学与生态学1区Top2014, 481, 392– 400, DOI: 10.1016/j.scitotenv.2014.02.069 21https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC2cXmtVWlu70%253D&md5=cc25f743eb20af754605612b81b94ea0Occurrence and fate of ozonation by-products at a full-scale drinking water treatment plantPapageorgiou, A.; Voutsa, D.; Papadakis, N.Science of the Total Environment (2014), 481 (), 392-400CODEN: STENDL; ISSN:0048-9697. (Elsevier B.V.)Occurrence and fate of carbonyl compds. as ozonation byproducts at a full scale drinking water treatment plant (DWTP) were studied for 1 yr. Raw water and post-treatment samples (pre-ozonation, coagulation/flocculation, sand filtration, main ozonation, granular activated C filtration, chlorination) were collected monthly. Pre-ozonation formed carbonyl compds. at 67.3 ± 43.3 μg/L as the sum of 14 carbonyl compds.; lower concns. were detd. following the main ozonation process, 32.8 ± 22.3 μg/L. Dominant compds. were formaldehyde, acetaldehyde, glyoxal, and Me glyoxal, contributing 65% of total carbonyl content. Dissolved org. C reactivity for carbonyl compd. formation varied throughout the year, exhibiting higher values in spring. Coagulation/flocculation and sand filtration significantly removed (64-80%) carbonyl compds. formed in the pre-ozonation step. Granular activated C filtration removal efficiency exhibited great variation, 15-62%. Carbonyl compd. concns. in finished water were low, close to detection limits, showed the efficiency of DWTP in removing this class of ozonation byproducts.
- 22Sun, W.; Lu, Z.; Zhang, Z.; Zhang, Y.; Shi, B.; Wang, H. Ozone and fenton oxidation affected the bacterial community and opportunistic pathogens in biofilms and effluents from GAC. Water Res.IF 12.8SCIEJCI 2.15Q1环境科学与生态学1区Top2022, 218, 118495, DOI: 10.1016/j.watres.2022.118495 There is no corresponding record for this reference.
- 23Ratzke, C.; Barrere, J.; Gore, J. Strength of species interactions determines biodiversity and stability in microbial communities. Nat. Ecol. Evol.IF 16.8SCIEJCI 3.93Q1生物学1区Top2020, 4, 376– 383, DOI: 10.1038/s41559-020-1099-4 23https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A280%3ADC%252BB387gsFWqtA%253D%253D&md5=1300026b85935909ddb38ad2b9172093Strength of species interactions determines biodiversity and stability in microbial communitiesRatzke Christoph; Barrere Julien; Gore Jeff; Barrere JulienNature ecology & evolution (2020), 4 (3), 376-383 ISSN:.Organisms-especially microbes-tend to live together in ecosystems. While some of these ecosystems are very biodiverse, others are not, and while some are very stable over time, others undergo strong temporal fluctuations. Despite a long history of research and a plethora of data, it is not fully understood what determines the biodiversity and stability of ecosystems. Theory and experiments suggest a connection between species interaction, biodiversity and the stability of ecosystems, where an increase in ecosystem stability with biodiversity could be observed in several cases. However, what causes these connections remains unclear. Here, we show in microbial ecosystems in the laboratory that the concentrations of available nutrients can set the strength of interactions between bacteria. High nutrient concentrations allowed the bacteria to strongly alter the chemical environment, causing on average more negative interactions between species. These stronger interactions excluded more species from the community, resulting in a loss of biodiversity. At the same time, the stronger interactions also decreased the stability of the microbial communities, providing a mechanistic link between species interaction, biodiversity and stability in microbial ecosystems.
- 24Desmond, P.; Best, J. P.; Morgenroth, E.; Derlon, N. Linking composition of extracellular polymeric substances (EPS) to the physical structure and hydraulic resistance of membrane biofilms. Water Res.IF 12.8SCIEJCI 2.15Q1环境科学与生态学1区Top2018, 132, 211– 221, DOI: 10.1016/j.watres.2017.12.058 24https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC1cXntlGntg%253D%253D&md5=8ad69e3d237d15096e8844ad9229fcc5Linking composition of extracellular polymeric substances (EPS) to the physical structure and hydraulic resistance of membrane biofilmsDesmond, Peter; Best, James P.; Morgenroth, Eberhard; Derlon, NicolasWater Research (2018), 132 (), 211-221CODEN: WATRAG; ISSN:0043-1354. (Elsevier Ltd.)The effect of extracellular polymeric substances (EPS) on the meso-scale phys. structure and hydraulic resistance of membrane biofilms during gravity driven membrane (GDM) filtration was investigated. Biofilms were developed on the surface of ultrafiltration membranes during dead-end filtration at ultra-low pressure (70mbar). Biofilm EPS compn. (total protein, polysaccharide and eDNA) was manipulated by growing biofilms under contrasting nutrient conditions. Nutrient conditions consisted of (i) a nutrient enriched condition with a nutrient ratio of 100:30:10 (C: N: P), (ii) a phosphorus limitation (C: N: P ratio: 100:30:0), and (iii) a nitrogen limitation (C: N: P ratio: 100:0:10). The structure of the biofilm was characterised at meso-scale using Optical Coherence Tomog. (OCT). Biofilm compn. was analyzed with respect to total org. carbon, total cellular mass and extracellular concns. of proteins, polysaccharides, and eDNA. 2D-confocal Raman mapping was used to characterize the functional group compn. and micro-scale distribution of the biofilms EPS. Our study reveals that the compn. of the EPS matrix can det. the meso-scale phys. structure of membrane biofilms and in turn its hydraulic resistance. Biofilms grown under P limiting conditions were characterised by dense and homogeneous phys. structures with high concns. of polysaccharides and eDNA. Biofilm grown under nutrient enriched or N limiting conditions were characterised by heterogeneous phys. structures with lower concns. of polysaccharides and eDNA. For P limiting biofilms, 2D-confocal Raman microscopy revealed a homogeneous spatial distribution of anionic functional groups in homogeneous biofilm structures with higher polysaccharide and eDNA concns. This study links EPS compn., phys. structure and hydraulic resistance of membrane biofilms, with practical relevance for the hydraulic performances of GDM ultrafiltration.
- 25Desmond, P.; Morgenroth, E.; Derlon, N. Physical structure determines compression of membrane biofilms during gravity driven membrane (GDM) ultrafiltration. Water Res.IF 12.8SCIEJCI 2.15Q1环境科学与生态学1区Top2018, 143, 539– 549, DOI: 10.1016/j.watres.2018.07.008 There is no corresponding record for this reference.
- 26Zhang, L.; Graham, N.; Derlon, N.; Tang, Y.; Siddique, M. S.; Xu, L.; Yu, W. Biofouling by ultra-low pressure filtration of surface water: The paramount role of initial available biopolymers. J. Membr. Sci.IF 9.5SCIEJCI 1.85Q1工程技术1区Top2021, 640, 119740, DOI: 10.1016/j.memsci.2021.119740 26https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BB3MXhvFCrt77O&md5=3e8eab80565dce0b9576d35cd0537559Biofouling by ultra-low pressure filtration of surface water: The paramount role of initial available biopolymersZhang, Li; Graham, Nigel; Derlon, Nicolas; Tang, Youneng; Siddique, Muhammad Saboor; Xu, Lei; Yu, WenzhengJournal of Membrane Science (2021), 640 (), 119740CODEN: JMESDO; ISSN:0376-7388. (Elsevier B.V.)Biofouling layer (i.e., biofilm) is an inevitable presence for the membrane filtration processes. In this study, we elucidated biofouling formation from the perspective of affecting the attachment of bacteria for the first time, whereby the role of initial available biopolymers was revealed. Results demonstrated that the presence of initial available biopolymers increased the abundance of the genus Caulobacter, which was capable of mineralizing biopolymers; whereas, for the typically oligotrophic species of Polynucleobacter, it exhibited low abundance. Greater concns. of polysaccharides and proteins were accumulated in the biofouling layer, when provided with initial biopolymers, and the biofilm structure was more heterogeneous with larger pore size and higher thickness. Thereby, the corresponding filtration system exhibited greater permeability and better removal performance of orgs. Collectively, the initial available biopolymers altered the attachment conditions for the bacteria, which subsequently impacted the bacterial community, and in turn biofilm compn., phys. structure and filtration performance.
- 27Tanentzap, A. J.; Fitch, A.; Orland, C.; Emilson, E. J. S.; Yakimovich, K. M.; Osterholz, H.; Dittmar, T. Chemical and microbial diversity covary in fresh water to influence ecosystem functioning. Proc. Natl. Acad. Sci. U.S.A.IF 11.1SCIEJCI 2.52Q1综合性期刊1区Top2019, 116 (49), 24689– 24695, DOI: 10.1073/pnas.1904896116 27https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC1MXitlejsLrM&md5=32a8b202a055c153ca8e479212707fd9Chemical and microbial diversity covary in fresh water to influence ecosystem functioningTanentzap, Andrew J.; Fitch, Amelia; Orland, Chloe; Emilson, Erik J. S.; Yakimovich, Kurt M.; Osterholz, Helena; Dittmar, ThorstenProceedings of the National Academy of Sciences of the United States of America (2019), 116 (49), 24689-24695CODEN: PNASA6; ISSN:0027-8424. (National Academy of Sciences)Invisible to the naked eye lies a tremendous diversity of org. mols. and organisms that make major contributions to important biogeochem. cycles. However, how the diversity and compn. of these two communities are interlinked remains poorly characterized in fresh waters, despite the potential for chem. and microbial diversity to promote one another. Here we exploited gradients in chemodiversity within a common microbial pool to test how chem. and biol. diversity covary and characterized the implications for ecosystem functioning. We found that both chemodiversity and genes assocd. with org. matter decompn. increased as more plant litterfall accumulated in exptl. lake sediments, consistent with scenarios of future environmental change. Chem. and microbial diversity were also pos. correlated, with dissolved org. matter having stronger effects on microbes than vice versa. Under our exptl. scenarios that increased sediment org. matter from 5 to 25% or darkened overlying waters by 2.5 times, the resulting increases in chemodiversity could increase greenhouse gas concns. in lake sediments by an av. of 1.5 to 2.7 times, when all of the other effects of litterfall and water color were considered. Our results open a major new avenue for research in aquatic ecosystems by exposing connections between chem. and microbial diversity and their implications for the global carbon cycle in greater detail than ever before.
- 28Judd, K. E.; Crump, B. C.; Kling, G. W. Variation in dissolved organic matter controls bacterial production and community composition. EcologyIF 4.8SCIEJCI 1.3Q1环境科学与生态学2区Top2006, 87 (8), 2068– 2079, DOI: 10.1890/0012-9658(2006)87[2068:VIDOMC]2.0.CO;2 28https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A280%3ADC%252BD28rhtl2gsg%253D%253D&md5=40a3ee97588aeb824b803be4f9437133Variation in dissolved organic matter controls bacterial production and community compositionJudd Kristin E; Crump Byron C; Kling George WEcology (2006), 87 (8), 2068-79 ISSN:0012-9658.An ongoing debate in ecology revolves around how species composition and ecosystem function are related. To address the mechanistic controls of this relationship, we manipulated the composition of dissolved organic matter (DOM) fed to aquatic bacteria to determine effects on both bacterial activity and community composition. Sites along terrestrial to aquatic flow paths were chosen to simulate movement of DOM through catchments, and DOM was fed to downslope and control bacterial communities. Bacterial production was measured, and DOM chemistry and bacterial community composition (using denaturing gradient gel electrophoresis of 16S rRNA genes) were characterized following incubations. Bacterial production, dissolved organic carbon (DOC)-specific bacterial production, and DOC consumption were greatest in mesocosms fed soil water DOM; soil water DOM enhanced lake and stream bacterial production by 320-670% relative to lake and stream controls. Stream DOM added to lake bacteria depressed bacterial production relative to lake controls in the early season (-78%) but not the mid-season experiment. Addition of upslope DOM to stream and lake bacterial communities resulted in significant changes in bacterial community composition relative to controls. In four of five DOM treatments, the bacterial community composition converged to the DOM source community regardless of the initial inoculum. These results demonstrate that shifts in the supply of natural DOM were followed by changes in both bacterial production and community composition, suggesting that changes in function are likely predicated on at least an initial change in the community composition. The results indicate that variation in DOM composition of soil and surface waters influences bacterial community dynamics and controls rates of carbon processing in set patterns across the landscape.
- 29Logue, J. B.; Stedmon, C. A.; Kellerman, A. M.; Nielsen, N. J.; Andersson, A. F.; Laudon, H.; Lindstrom, E. S.; Kritzberg, E. S. Experimental insights into the importance of aquatic bacterial community composition to the degradation of dissolved organic matter. ISME J.IF 11.0SCIEJCI 2.59Q1环境科学与生态学1区Top2016, 10 (3), 533– 545, DOI: 10.1038/ismej.2015.131 29https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC28XjtFKrsb0%253D&md5=6b5000920df98fcaea68d8158f5886a7Experimental insights into the importance of aquatic bacterial community composition to the degradation of dissolved organic matterLogue, Jurg B.; Stedmon, Colin A.; Kellerman, Anne M.; Nielsen, Nikoline J.; Andersson, Anders F.; Laudon, Hjalmar; Lindstroem, Eva S.; Kritzberg, Emma S.ISME Journal (2016), 10 (3), 533-545CODEN: IJSOCF; ISSN:1751-7362. (Nature Publishing Group)Bacteria play a central role in the cycling of carbon, yet our understanding of the relationship between the taxonomic compn. and the degrdn. of dissolved org. matter (DOM) is still poor. In this exptl. study, we were able to demonstrate a direct link between community compn. and ecosystem functioning in that differently structured aquatic bacterial communities differed in their degrdn. of terrestrially derived DOM. Although the same amt. of carbon was processed, both the temporal pattern of degrdn. and the compds. degraded differed among communities. We, moreover, uncovered that low-mol.-wt. carbon was available to all communities for utilization, whereas the ability to degrade carbon of greater mol. wt. was a trait less widely distributed. Finally, whereas the degrdn. of either low- or high-mol.-wt. carbon was not restricted to a single phylogenetic clade, our results illustrate that bacterial taxa of similar phylogenetic classification differed substantially in their assocn. with the degrdn. of DOM compds. Applying techniques that capture the diversity and complexity of both bacterial communities and DOM, our study provides new insight into how the structure of bacterial communities may affect processes of biogeochem. significance.
- 30Kujawinski, E. B. The impact of microbial metabolism on marine dissolved organic matter. Annu. Rev. Mar. Sci.IF 17.3SCIEJCI 2.47Q1地球科学1区Top2011, 3, 567– 599, DOI: 10.1146/annurev-marine-120308-081003 30https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A280%3ADC%252BC3M3gtlKrtQ%253D%253D&md5=f7bd65b5ad6db4014b202d175dcb6f89The impact of microbial metabolism on marine dissolved organic matterKujawinski Elizabeth BAnnual review of marine science (2011), 3 (), 567-99 ISSN:1941-1405.Microbes mediate global biogeochemical cycles through their metabolism, and all metabolic processes begin with the interaction between the microbial cell wall or membrane and the external environment. For all heterotrophs and many autotrophs, critical growth substrates and factors are present within the dilute and heterogeneous mixture of compounds that constitutes dissolved organic matter (DOM). In short, the microbe-molecule interaction is one of the fundamental reactions within the global carbon cycle. Here, I summarize recent findings from studies that examine DOM-microbe interactions from either the DOM perspective (organic geochemistry) or the microbe perspective (microbial ecology). Gaps in our knowledge are highlighted and future integrative research directions are proposed.
- 31Osterholz, H.; Singer, G.; Wemheuer, B.; Daniel, R.; Simon, M.; Niggemann, J.; Dittmar, T. Deciphering associations between dissolved organic molecules and bacterial communities in a pelagic marine system. ISME J.IF 11.0SCIEJCI 2.59Q1环境科学与生态学1区Top2016, 10 (7), 1717– 1730, DOI: 10.1038/ismej.2015.231 31https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC28XhtVahu7fN&md5=253c21d9b747758f1b6733dd9f721a3eDeciphering associations between dissolved organic molecules and bacterial communities in a pelagic marine systemOsterholz, Helena; Singer, Gabriel; Wemheuer, Bernd; Daniel, Rolf; Simon, Meinhard; Niggemann, Jutta; Dittmar, ThorstenISME Journal (2016), 10 (7), 1717-1730CODEN: IJSOCF; ISSN:1751-7362. (Nature Publishing Group)Dissolved org. matter (DOM) is the main substrate and energy source for heterotrophic bacterioplankton. To understand the interactions between DOM and the bacterial community (BC), it is important to identify the key factors on both sides in detail, chem. distinct moieties in DOM and the various bacterial taxa. Next-generation sequencing facilitates the classification of millions of reads of environmental DNA and RNA amplicons and ultrahigh-resoln. mass spectrometry yields up to 10 000 DOM mol. formulas in a marine water sample. Linking this detailed biol. and chem. information is a crucial first step toward a mechanistic understanding of the role of microorganisms in the marine carbon cycle. In this study, we interpreted the complex microbiol. and mol. information via a novel combination of multivariate statistics. We were able to reveal distinct relationships between the key factors of org. matter cycling along a latitudinal transect across the North Sea. Total BC and DOM compn. were mainly driven by mixing of distinct water masses and presumably retain their resp. terrigenous imprint on similar timescales on their way through the North Sea. The active microbial community, however, was rather influenced by local events and correlated with specific DOM mol. formulas indicative of compds. that are easily degradable. These trends were most pronounced on the highest resolved level, i.e., operationally defined 'species', reflecting the functional diversity of microorganisms at high taxonomic resoln. Sequence data were deposited inthe Sequence Read Archive (SRA) of the National Center for Biotechnol. Information (NCBI) under the accession no. SRA082674.
- 32Bader, H. Determination of ozone in water by the indigo method: A submitted standard method. Ozone: Sci. Eng.IF 2.7SCIEJCI 0.32Q3环境科学与生态学4区1982, 4 (4), 169– 176, DOI: 10.1080/01919518208550955 32https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADyaL3sXksVeitLg%253D&md5=f077fd7064dc297741a9c0c09f725531Determination of ozone in water by the indigo method; a submitted standard methodBader, H.; Hoigne, J.Ozone: Science & Engineering (1982), 4 (4), 169-76CODEN: OZSEDS; ISSN:0191-9512.A selective and simple method for the detn. of O3, as formulated for the new Swiss Std. Methods for drinking water anal., is presented. O3 rapidly and stoichiometrically decolorizes tri-K indigo trisulfonate [67627-18-3] in acidic soln. The decrease in absorbance at 600 nm is linear with O3 residual and is 0.42 ± 0.01/cm per mg/L. The limits of detection are 2 μg μg/L for an instrumental and 10 mg/L for a visual field method.
- 33Dittmar, T.; Koch, B.; Hertkorn, N.; Kattner, G. A simple and efficient method for the solid-phase extraction of dissolved organic matter (SPE-DOM) from seawater. Limnol. Oceanogr.: MethodsIF 2.7SCIEJCI 0.84Q2地球科学3区2008, 6, 230– 235, DOI: 10.4319/lom.2008.6.230 33https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BD1cXhtlOnt7jI&md5=3f114d54f73464b3c5dc217c5fd7790eA simple and efficient method for the solid-phase extraction of dissolved organic matter (SPE-DOM) from seawaterDittmar, Thorsten; Koch, Boris; Hertkorn, Norbert; Kattner, GerhardLimnology and Oceanography: Methods (2008), 6 (June), 230-235CODEN: LOMIBY; ISSN:1541-5856. (American Society of Limnology and Oceanography)A simple protocol is presented for the solid-phase extn. of dissolved org. matter (SPE-DOM) from seawater using com. prepacked cartridges. The method does not require major instrumentation and can be performed in the field. Modified styrene divinyl benzene polymer type sorbents (Varian PPL and ENV) and sorbents of a silica structure bonded with different hydrocarbon chains (Varian C8, C18, C18OH, and C18EWP) were considered. Except for C18OH, which heavily contaminated the samples, none of the sorbents leached significant amts. of dissolved org. carbon (DOC) or nitrogen (DON). Samples from the North Brazil shelf with strong mixing gradients of terrigenous and marine DOM were used to compare the various sorbents. PPL was the most efficient-on av., 62% of DOC was recovered as salt-free exts. C18 was found to be most efficient among the silica-based sorbents, but it showed only two-thirds of the extn. efficiency of PPL. As indicated by [1H]NMR, C/N, and δ13C analyses, PPL extd. a more representative proportion of DOM than C18. Therefore, PPL was used for comparative studies in the Gulf of Mexico and Antarctica. From brackish marsh and river waters, 65% and 62% of total DOC, resp., could be extd. For purely marine DOM in Antarctica and the deep sea, the extn. efficiency was lower (43% on av.). The efficiency of the new method to isolate marine DOM is better than or similar to highly laborious methods. A further advantage is the complete desalination of the sample. The isolation of a major DOM fraction, which is salt-free, offers many possibilities to further characterize DOM by advanced anal. techniques.
- 34Li, F.; Tang, S.; Lv, J.; He, A.; Wang, Y.; Liu, S.; Cao, H.; Zhao, L.; Wang, Y.; Jiang, G. Molecular-scale investigation on the formation of brown carbon aerosol via iron-phenolic compound reactions in the dark. Environ. Sci. Technol.IF 11.4SCIEJCI 1.44Q1环境科学与生态学1区Top2023, 57 (30), 11173– 11184, DOI: 10.1021/acs.est.3c04263 There is no corresponding record for this reference.
- 35Zherebker, A.; Shirshin, E.; Rubekina, A.; Kharybin, O.; Kononikhin, A.; Kulikova, N. A.; Zaitsev, K. V.; Roznyatovsky, V. A.; Grishin, Y. K.; Perminova, I. V.; Nikolaev, E. N. Optical properties of soil dissolved organic matter are related to acidic functions of its components as revealed by fractionation, selective deuteromethylation, and ultrahigh resolution mass spectrometry. Environ. Sci. Technol.IF 11.4SCIEJCI 1.44Q1环境科学与生态学1区Top2020, 54 (5), 2667– 2677, DOI: 10.1021/acs.est.9b05298 35https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BB3cXislartb0%253D&md5=b4eb098cd023482ec11f33b75fd25fa6Optical Properties of Soil Dissolved Organic Matter Are Related to Acidic Functions of Its Components as Revealed by Fractionation, Selective Deuteromethylation, and Ultrahigh Resolution Mass SpectrometryZherebker, Alexander; Shirshin, Evgeny; Rubekina, Anna; Kharybin, Oleg; Kononikhin, Alexey; Kulikova, Natalia A.; Zaitsev, Kirill V.; Roznyatovsky, Vitaliy A.; Grishin, Yuri K.; Perminova, Irina V.; Nikolaev, Evgeny N.Environmental Science & Technology (2020), 54 (5), 2667-2677CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)The goal of this study was to establish a relationship between the optical properties of soil dissolved org. matter (DOM) and acidic functions carried out by its individual constituents. We obtained 12 fractions of DOM samples using sequential solid phase extn. on nonionic sorbent at steadily lowered pH values: 7, 5, 3, 2, which correspond to low bounds of pKa values of phenols, aliph., and arom. carboxylic acids, and ketoacids. The structural studies were conducted with the use of NMR and selective deuteromethylation of isolated fractions coupled to ultrahigh resoln. mass spectrometry. First, a gradual shift of mol. compns. was obsd. from reduced components to arom. oxidized compds. isolated at pH 7 and 2, resp. Changes in mol. compns. were accompanied by a red shift of fluorescence spectra. Further application of deuteromethylation enabled us to distinguish DOM constituents with different amts. of carboxylic groups. Moreover, identification of structural isomers in a single DOM sample was achieved. Statistical anal. revealed that red shift of fluorescence is facilitated by the increase of a contribution of arom. poly(carboxylic acid)s with high conjugation lengths. Addnl., anal. of the labeled fractionated permafrost thaw DOM directly showed carboxyl-rich alicyclic mols., while the same components from lower-latitude DOM were assigned to lignin-like species.
- 36Lv, J. T.; Zhang, S. Z.; Wang, S. S.; Luo, L.; Cao, D.; Christie, P. Molecular-scale investigation with ESI-FT-ICR-MS on fractionation of dissolved organic matter induced by adsorption on iron oxyhydroxides. Environ. Sci. Technol.IF 11.4SCIEJCI 1.44Q1环境科学与生态学1区Top2016, 50 (5), 2328– 2336, DOI: 10.1021/acs.est.5b04996 36https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC28XhsVymsrg%253D&md5=41055937d3e93d140dfa0e258cbd8fa5Molecular-Scale Investigation with ESI-FT-ICR-MS on Fractionation of Dissolved Organic Matter Induced by Adsorption on Iron OxyhydroxidesLv, Jitao; Zhang, Shuzhen; Wang, Songshan; Luo, Lei; Cao, Dong; Christie, PeterEnvironmental Science & Technology (2016), 50 (5), 2328-2336CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)Adsorption by minerals is a common geochem. process of dissolved org. matter (DOM) which may induce fractionation of DOM at the mineral-water interface. We examine the mol. fractionation of DOM induced by adsorption onto 3 common iron oxyhydroxides using electrospray ionization coupled with Fourier-transform ion cyclotron resonance mass spectrometry (ESI-FT-ICR-MS). Ferrihydrite exhibited higher affinity to DOM and induced more pronounced mol. fractionation of DOM than did goethite or lepidocrocite. High mol. wt. (>500 Da) compds. and compds. high in unsatn. or rich in O including polycyclic aroms., polyphenols and carboxylic compds. had higher affinity to Fe oxyhydroxides and esp. to ferrihydrite. Low mol. wt. compds. and compds. low in unsatn. or contg. few oxygenated groups (mainly alcs. and ethers) were preferentially maintained in soln. This study confirms that the double bond equivalence and the no. of O atoms are valuable parameters indicating the selective fractionation of DOM at mineral and water interfaces. The results provide important information for further understanding the behavior of DOM in the natural environment.
- 37Yu, S.; Lv, J.; Jiang, L.; Geng, P.; Cao, D.; Wang, Y. Changes of soil dissolved organic matter and its relationship with microbial community along the Hailuogou Glacier forefield chronosequence. Environ. Sci. Technol.IF 11.4SCIEJCI 1.44Q1环境科学与生态学1区Top2023, 57 (9), 4027– 4038, DOI: 10.1021/acs.est.2c08855 37https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BB3sXjsF2ku70%253D&md5=2027aea4128a32032070ee402ce859cdChanges of Soil Dissolved Organic Matter and Its Relationship with Microbial Community along the Hailuogou Glacier Forefield ChronosequenceYu, Shiyang; Lv, Jitao; Jiang, Lu; Geng, Pengyu; Cao, Dong; Wang, YaweiEnvironmental Science & Technology (2023), 57 (9), 4027-4038CODEN: ESTHAG; ISSN:1520-5851. (American Chemical Society)Glacier-retreated areas are ideal areas to study soil biogeochem. processes during vegetation succession, because of the limited effect of other environmental and climatic factors. In this study, the changes of soil dissolved org. matter (DOM) and its relationship with microbial communities along the Hailuogou Glacier forefield chronosequence were investigated. Both microbial diversity and DOM mol. chemodiversity recovered rapidly at the initial stage, indicating the pioneering role of microorganisms in soil formation and development. The chem. stability of soil org. matter enhanced with vegetation succession due to the retaining of compds. with high oxidn. state and aromaticity. The mol. compn. of DOM affected microbial communities, while microorganisms tended to utilize labile components to form refractory components. This complex relationship network between microorganisms and DOM components played an important role in the development of soil org. matter as well as the formation of stable soil carbon pool in glacier-retreated areas.
- 38Lv, J.; Miao, Y.; Huang, Z.; Han, R.; Zhang, S. Facet-mediated adsorption and molecular fractionation of humic substances on hematite surfaces. Environ. Sci. Technol.IF 11.4SCIEJCI 1.44Q1环境科学与生态学1区Top2018, 52 (20), 11660– 11669, DOI: 10.1021/acs.est.8b03940 38https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC1cXhslantbzF&md5=a7f01e37d9f34127ca60d39cdd847990Facet-Mediated Adsorption and Molecular Fractionation of Humic Substances on Hematite SurfacesLv, Jitao; Miao, Yuexia; Huang, Zaoquan; Han, Ruixia; Zhang, ShuzhenEnvironmental Science & Technology (2018), 52 (20), 11660-11669CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)Interactions between dissolved org. matter (DOM) and iron oxyhydroxides have important environmental and geochem. implications. The present study employed two hematite nanocrystals to investigate the adsorption and mol. fractionation of two typical humic substances (HSs) using electrospray ionization coupled with Fourier transform ion cyclotron resonance mass spectrometry (ESI-FT-ICR-MS). Hematite with a predominant exposure of {100} facets induced more pronounced adsorption and mol. fractionation of HSs than {001} facets, indicating that the interfacial adsorptive fractionation process of HSs was mediated by exposed facets of hematite. Further exploration of the surface OH groups of the two hematite nanocrystals confirms that the facet-mediated mol. fractionation of HSs was attributable to the abundance of singly iron-atom coordinated -OH sites on the hematite surfaces. Mols. with a high oxidn. state and high aromaticity such as oxidized black carbon, polyphenol-like, and tannic-like compds. preferentially formed ligand-exchange complexes with singly coordinated -OH groups on the hematite surfaces, inducing the selective binding and mol. fractionation of HSs at the mineral-water interface. These results demonstrate that singly iron-atom coordinated -OH sites det. DOM adsorption and mediate mol. fractionation on hematite surfaces, and this contributes substantially to our understanding of the mol. mechanisms of iron oxyhydroxide-mediated mol. exchange of DOM in soils and/or sediments.
- 39Koch, B. P.; Dittmar, T.; Witt, M.; Kattner, G. Fundamentals of molecular formula assignment to ultrahigh resolution mass data of natural organic matter. Anal. Chem.IF 7.4SCIEJCI 1.71Q1化学1区Top2007, 79 (4), 1758– 1763, DOI: 10.1021/ac061949s 39https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BD2sXjtVahtg%253D%253D&md5=b296c368a5fbeb290a77e549ec58487bFundamentals of molecular formula assignment to ultrahigh resolution mass data of natural organic matterKoch, Boris P.; Dittmar, Thorsten; Witt, Matthias; Kattner, GerhardAnalytical Chemistry (2007), 79 (4), 1758-1763CODEN: ANCHAM; ISSN:0003-2700. (American Chemical Society)Ultrahigh-resoln. mass spectrometry via the Fourier transform ICR technique (FT-ICR-MS) allows the identification of thousands of different mol. formulas in natural org. matter and petroleum samples. Mol. formula assignment from mass data is most crit. and time-consuming for these samples, and in many cases, several formulas can be detd. for the same mol. mass. Therefore, automated procedures are required for an efficient exploitation of the extensive data sets. Here, the authors revise statements in a recent publication, which might result in a misleading impression about the authors' approach of formula assignment in a previous work. The authors also summarize and categorize existing procedures for formula assignment. The authors propose new techniques, which are suitable to be implemented in automated evaluation software. The homologous series approach is extended toward a building block approach that can be applied as a new exclusion criterion for incorrect formula assignments. The examn. of stable isotope ratios of individual mols. in natural org. matter can be applied as an addnl. and intrinsic evaluation for calcd. mol. formulas.
- 40Sun, K.; Han, L. F.; Yang, Y.; Xia, X. H.; Yang, Z. F.; Wu, F. C.; Li, F. B.; Feng, Y. F.; Xing, B. S. Application of hydrochar altered soil microbial community composition and the molecular structure of native soil organic carbon in a paddy soil. Environ. Sci. Technol.IF 11.4SCIEJCI 1.44Q1环境科学与生态学1区Top2020, 54 (5), 2715– 2725, DOI: 10.1021/acs.est.9b05864 40https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BB3cXitFejsrY%253D&md5=a50ee46c2ba85eb40d5b47850626c3f8Application of Hydrochar Altered Soil Microbial Community Composition and the Molecular Structure of Native Soil Organic Carbon in a Paddy SoilSun, Ke; Han, Lanfang; Yang, Yan; Xia, Xinghui; Yang, Zhifeng; Wu, Fengchang; Li, Fangbai; Feng, Yanfang; Xing, BaoshanEnvironmental Science & Technology (2020), 54 (5), 2715-2725CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)The benefits and disadvantages of hydrochar incorporation into soil have been heavily researched. However, the effect of hydrochar application on the soil microbial communities and the mol. structure of native soil org. carbon (SOC) has not been thoroughly elucidated. This study conducted an incubation expt. at 25°C for 135 days using a soil column with 0.5 and 1.5% hydrochar-amended paddy soil to explore the interconnections between changes in soil properties and microbial communities and shifts in native SOC structure using electrospray ionization Fourier transform ion cyclotron resonance mass spectrometry (ESI-FT-ICR-MS) and NMR after hydrochar application. Hydrochar addn. decreased the labile SOC fraction by 15.6-33.6% and increased the stable SOC fraction by 10.3-27.0%. These effects were significantly stronger for 1.5% hydrochar-treated soil. Addnl., hydrochar addn. induced the native SOC with 1.0-3.0% more carbon and 6.0-13.0% higher mol. wt. The SOC in hydrochar-amended soil contained more arom. compds. but fewer carbohydrates and lower polarity. This was resulted by a statistically significant redn. in Sphingobacterium, which was active in polycyclic arom. hydrocarbon degrdn., and an increase in Flavobacterium, Anaerolinea, Penicillium, and Acremonium, which were the efficient decomposers of labile SOC. These findings will help elucidate the potential influence of hydrochar on the carbon biogeochem. cycle in the soil.
- 41Koch, B. P.; Dittmar, T. From mass to structure: An aromaticity index for high-resolution mass data of natural organic matter. Rapid Commun. Mass Spectrom.IF 2.0SCIEJCI 0.65Q3化学3区2006, 20 (5), 926– 932, DOI: 10.1002/rcm.2386 41https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BD28XitlGgs74%253D&md5=86bf95387b3e6f752481d4f026cbd184From mass to structure: an aromaticity index for high-resolution mass data of natural organic matterKoch, B. P.; Dittmar, T.Rapid Communications in Mass Spectrometry (2005), 20 (5), 926-932CODEN: RCMSEF; ISSN:0951-4198. (John Wiley & Sons Ltd.)Recent progress in Fourier transform ion cyclotron resonance mass spectrometry (FTICRMS) has provided extensive mol. mass data for complex natural org. matter (NOM). Structural information can be deduced solely from the mol. masses for ions with extreme mol. element ratios, in particular low H/C ratios, which are abundant in thermally altered NOM (e.g. black carbon). In this communication we propose a general aromaticity index (AI) and two threshold values as unequivocal criteria for the existence of either arom. (AI > 0.5) or condensed arom. structures (AI ≥ 0.67) in NOM. AI can be calcd. from mol. formulas which are derived from exact mol. masses of naturally occurring compds. contg. C, H, O, N, S and P, and is esp. useful for substances with arom. cores and few alkylations. In order to test the validity of our model index, AI is applied to FTICRMS data of a NOM deep-water sample from the Weddell Sea (Antarctica), a fulvic acid std., and an artificial dataset of all theor. possible mol. formulas. For graphical evaluation a ternary plot is suggested for four-dimensional data representation. The proposed aromaticity index is a step towards structural identification of NOM and the mol. identification of polyarom. hydrocarbons in the environment.
- 42Ding, Y.; Shi, Z. Q.; Ye, Q. T.; Liang, Y. Z.; Liu, M. Q.; Dang, Z.; Wang, Y. J.; Liu, C. X. Chemodiversity of soil dissolved organic matter. Environ. Sci. Technol.IF 11.4SCIEJCI 1.44Q1环境科学与生态学1区Top2020, 54 (10), 6174– 6184, DOI: 10.1021/acs.est.0c01136 42https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BB3cXntl2ku74%253D&md5=753cd5d70afbd947afb7d847cb39bc0aChemodiversity of Soil Dissolved Organic MatterDing, Yang; Shi, Zhenqing; Ye, Qianting; Liang, Yuzhen; Liu, Minqin; Dang, Zhi; Wang, Yujun; Liu, ChongxuanEnvironmental Science & Technology (2020), 54 (10), 6174-6184CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)Dissolved org. matter (DOM) plays a key role in many biogeochem. processes, but the drivers controlling the diversity of chem. compn. and properties of DOM mols. (chemodiversity) in soils are poorly understood. It has also been debated whether environmental conditions or intrinsic mol. properties control the accumulation and persistence of DOM due to the complexity of both mol. compn. of DOM and interactions between DOM and surrounding environments. Soil DOM samples were extd. from 33 soils collected from different regions of China, and we studied the effects of climate and soil properties on the chemodiversity of DOM across different regions of China, employing a combination of Fourier transform ICR mass spectrometry, optical spectroscopy, and statistical analyses. Despite the heterogeneity of soil samples and complex influencing factors, aridity and clay can account for the majority of the variations of DOM chem. compn. The finding implied that DOM chemodiversity is an ecosystem property closely related to the environment, and can be used in developing large-scale soil biogeochem. models for predicting C cycling in soils.
- 43Lawaetz, A. J.; Stedmon, C. A. Fluorescence intensity calibration using the Raman scatter peak of water. Appl. Spectrosc.IF 3.5SCIEJCI 0.91Q1化学3区2009, 63 (8), 936– 940, DOI: 10.1366/000370209788964548 43https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BD1MXhtVaht7fM&md5=9b276ac6eb08dda3e51c3f158d5c287eFluorescence intensity calibration using the Raman scatter peak of waterLawaetz, A. J.; Stedmon, C. A.Applied Spectroscopy (2009), 63 (8), 936-940CODEN: APSPA4; ISSN:0003-7028. (Society for Applied Spectroscopy)Fluorescence data of replicate samples obtained from different fluorescence spectrometers or by the same spectrometer but with different instrument settings can have great intensity differences. To compare such data an intensity calibration must be applied. Here we explain a simple calibration method for fluorescence intensity using only the integrated area of a water Raman peak. By applying this method to data from three different instruments, we show that it is possible to remove instrument-dependent intensity factors, and we present results on a unified scale of Raman units. The method presented is a rapid and simple approach suitable for routine measurements with no need for hazardous chems.
- 44Gong, J.; Liu, Y.; Sun, X. O3 and UV/O3 oxidation of organic constituents of biotreated municipal wastewater. Water Res.IF 12.8SCIEJCI 2.15Q1环境科学与生态学1区Top2008, 42 (4–5), 1238– 1244, DOI: 10.1016/j.watres.2007.09.020 44https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BD1cXhvFyrtL4%253D&md5=915943a456b48176f79ca420443bf2f8O3 and UV/O3 oxidation of organic constituents of biotreated municipal wastewaterGong, Jianli; Liu, Yongdi; Sun, XianboWater Research (2008), 42 (4-5), 1238-1244CODEN: WATRAG; ISSN:0043-1354. (Elsevier Ltd.)Dissolved org. matter (DOM) in the biotreated effluent of a municipal wastewater treatment plant was sepd. by XAD-8 and XAD-4 resins into four fractions: hydrophobic acids, non-acid hydrophobics, transphilics and hydrophilics. Ozonation with and without UV enhancement removed most UV-absorbing substances in the first 30 min achieving 78% and 63% redn. in UV254, resp.; the UV enhancement resulted in a greater redn. in dissolved org. carbon (DOC) (90% vs. 36%). Ozone reacted sequentially with arom. hydrophobics, transphilics, and then hydrophilics; however, under UV, it reacted with all four org. fractions simultaneously. Low-MW hydrophilics were the most abundant fraction in the ozone-treated effluent.
- 45Ohno, T.; He, Z.; Sleighter, R. L.; Honeycutt, C. W.; Hatcher, P. G. Ultrahigh resolution mass spectrometry and indicator species analysis to identify marker components of soil- and plant biomass- derived organic matter fractions. Environ. Sci. Technol.IF 11.4SCIEJCI 1.44Q1环境科学与生态学1区Top2010, 44 (22), 8594– 8600, DOI: 10.1021/es101089t 45https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC3cXhtlShs7rK&md5=d82e6c5d259208b4b53548c6928c4453Ultrahigh Resolution Mass Spectrometry and Indicator Species Analysis to Identify Marker Components of Soil- and Plant Biomass-Derived Organic Matter FractionsOhno, Tsutomu; He, Zhongqi; Sleighter, Rachel L.; Honeycutt, C. Wayne; Hatcher, Patrick G.Environmental Science & Technology (2010), 44 (22), 8594-8600CODEN: ESTHAG; ISSN:0013-936X. (American Chemical Society)The chem. properties of org. matter affect important soil processes such as speciation, solubilization, and transport of plant nutrients and metals. This work uses ultrahigh resoln. electrospray ionization Fourier transform ion cyclotron resonance mass spectrometry to det. the mol. compn. of three org. matter fractions of soils and aq. exts. of crop biomass. Comparison of the van Krevelen plots allowed tracking the changes in org. matter with increasing humification. Aq. plant biomass exts. contain a diverse mixt. of lipids, proteins, and lignins. Soil aq. exts. were marked by increases in lignin and carbohydrate components and decrease in the protein component as compared to the plant ext. Refractory humic acid fractions were marked by decrease in the lignin component and increases in the lipid and condensed arom. components. The multivariate indicator species anal. was used to identify marker components of the four org. matter types investigated. The plant ext. group had 772 marker components compared to 237 for soil aq. ext., 92 for mobile humic acid, and 418 for calcium humic acid. This study demonstrates that ultrahigh resoln. mass spectrometry and multivariate methods can be used to identify marker components to gain a mol.-scale description and understanding of C dynamics.
- 46LaRowe, D. E.; Van Cappellen, P. Degradation of natural organic matter: A thermodynamic analysis. Geochim. Cosmochim. ActaIF 5.0SCIEJCI 1.52Q1地球科学1区Top2011, 75 (8), 2030– 2042, DOI: 10.1016/j.gca.2011.01.020 46https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC3MXjsVGhu78%253D&md5=3a0610f4c212fc480d02649866bfdffdDegradation of natural organic matter: A thermodynamic analysisLaRowe, Douglas E.; Van Cappellen, PhilippeGeochimica et Cosmochimica Acta (2011), 75 (8), 2030-2042CODEN: GCACAK; ISSN:0016-7037. (Elsevier B.V.)The oxidative degrdn. of org. matter is a key process in the biogeochem. functioning of the earth system. Quant. models of org. matter degrdn. are therefore essential for understanding the chem. state and evolution of the Earth's near-surface environment, and to forecast the biogeochem. consequences of ongoing regional and global change. The complex nature of biol. produced org. matter represents a major obstacle to the development of such models, however. The authors compare the energetics of the oxidative degrdn. of a large no. of naturally occurring org. compds. By relating the Gibbs energies of half reactions describing the complete mineralization of the compds. to their av. nominal carbon oxidn. state, it becomes possible to est. the energetic potential of the compds. based on major element (C, H, N, O, P, S) ratios. The new energetic description of org. matter can be combined with bioenergetic theory to rationalize obsd. patterns in the decompn. of natural org. matter. For example, the persistence of cell membrane derived compds. and complex orgs. in anoxic settings is consistent with their limited catabolic potential under these environmental conditions. The proposed approach opens the way to include the thermodn. properties of org. compds. in kinetic models of org. matter degrdn.
- 47Ribeirinho-Soares, S.; Moreira, N. F. F.; Graca, C.; Pereira, M. F. R.; Silva, A. M. T.; Nunes, O. C. Overgrowth control of potentially hazardous bacteria during storage of ozone treated wastewater through natural competition. Water Res.IF 12.8SCIEJCI 2.15Q1环境科学与生态学1区Top2022, 209, 117932, DOI: 10.1016/j.watres.2021.117932 47https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BB3MXislWku77M&md5=d2a523efc46f70766df13794f91f3681Overgrowth control of potentially hazardous bacteria during storage of ozone treated wastewater through natural competitionRibeirinho-Soares, Sara; Moreira, Nuno F. F.; Graca, Catia; Pereira, M. Fernando R.; Silva, Adrian M. T.; Nunes, Olga C.Water Research (2022), 209 (), 117932CODEN: WATRAG; ISSN:0043-1354. (Elsevier Ltd.)Improving the chem. and biol. quality of treated wastewater is particularly important in world regions under water stress. In these regions, reutilization of wastewater is seen as an alternative to reduce water demand, particularly for agriculture irrigation. In a reuse scenario, the treated wastewater must have enough quality to avoid chem. and biol. contamination of the receiving environment. Ozonation is among the technologies available to efficiently remove org. micropollutants and disinfect secondary effluents, being implemented in full-scale urban wastewater treatment plants worldwide. However, previous studies demonstrated that storage of ozone treated wastewater promoted the overgrowth of potentially harmful bacteria, putting at risk its reutilization, given for instance the possibility of contaminating the food-chain. Therefore, this study was designed to assess the potential beneficial role of inoculation of ozone treated wastewater with a diverse bacterial community during storage, for the control of the overgrowth of potentially hazardous bacteria, through bacterial competition. To achieve this goal, ozone treated wastewater (TWW) was dild. with river water (RW) in the same proportion, and the resulting bacterial community (RW+TWW) was compared to that of undiluted TWW over 7 days storage. As hypothesized, in contrast to TWW, where dominance of Beta- and Gammaproteobacteria, namely Pseudomonas spp. and Acinetobacter spp., was obsd. upon storage for 7 days, the bacterial communities of the dild. samples (RW+TWW) were diverse, resembling those of RW. Moreover, given the high abundance of antibiotic resistance genes in RW, the concn. of these genes in RW+TWW did not differ from that of the non-ozonated controls (WW, RW and RW+WW) over the storage period. These results highlight the necessity of finding a suitable pristine diverse bacterial community to be used in the future to compete with bacteria surviving ozonation, to prevent reactivation of undesirable bacteria during storage of treated wastewater.
- 48Rehman, Z. U.; Ali, M.; Iftikhar, H.; Leiknes, T. Genome-resolved metagenomic analysis reveals roles of microbial community members in full-scale seawater reverse osmosis plant. Water Res.IF 12.8SCIEJCI 2.15Q1环境科学与生态学1区Top2019, 149, 263– 271, DOI: 10.1016/j.watres.2018.11.012 There is no corresponding record for this reference.
- 49Wang, H.; Zhang, C.; Wang, Y.-N.; Sun, Y.; Fu, Y.; Gong, Z.; Liu, K. Simultaneous degradation of refractory organics, antibiotics and antibiotic resistance genes from landfill leachate concentrate by GAC/O3. J. Cleaner Prod.IF 11.1SCIEJCI 1.53Q1环境科学与生态学1区Top2022, 380, 135016, DOI: 10.1016/j.jclepro.2022.135016 There is no corresponding record for this reference.
- 50Tadonléké, R. D. Strong coupling between natural Planctomycetes and changes in the quality of dissolved organic matter in freshwater samples. FEMS Microbiol. Ecol.IF 4.2SCIEJCI 0.8Q2生物学3区2007, 59 (3), 543– 555, DOI: 10.1111/j.1574-6941.2006.00222.x There is no corresponding record for this reference.
- 51Nichols, G. L.; McLauchlin, J. Microbiology and the investigation of waterborne outbreaks: The use of Cryptosporidium typing in the investigation of waterborne disease. In Drinking Water and Infectious Disease: Establishing the Links; CRC Press, 2002, pp 87– 95. DOI: 10.1201/9781420040524.ch8 .There is no corresponding record for this reference.
- 52Lau, H. Y.; Ashbolt, N. J. The role of biofilms and protozoa in Legionella pathogenesis: Implications for drinking water. J. Appl. Microbiol.IF 4.0SCIEJCI 0.68Q2生物学3区2009, 107 (2), 368– 378, DOI: 10.1111/j.1365-2672.2009.04208.x 52https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A280%3ADC%252BD1MvptFWjtw%253D%253D&md5=c74d388e5e2f29221200d8b4ac872b8cThe role of biofilms and protozoa in Legionella pathogenesis: implications for drinking waterLau H Y; Ashbolt N JJournal of applied microbiology (2009), 107 (2), 368-78 ISSN:.Current models to study Legionella pathogenesis include the use of primary macrophages and monocyte cell lines, various free-living protozoan species and murine models of pneumonia. However, there are very few studies of Legionella spp. pathogenesis aimed at associating the role of biofilm colonization and parasitization of biofilm microbiota and release of virulent bacterial cell/vacuoles in drinking water distribution systems. Moreover, the implications of these environmental niches for drinking water exposure to pathogenic legionellae are poorly understood. This review summarizes the known mechanisms of Legionella spp. proliferation within Acanthamoeba and mammalian cells and advocates the use of the amoeba model to study Legionella pathogenicity because of their close association with Legionella spp. in the aquatic environment. The putative role of biofilms and amoebae in the proliferation, development and dissemination of potentially pathogenic Legionella spp. is also discussed. Elucidating the mechanisms of Legionella pathogenicity development in our drinking water systems will aid in elimination strategies and procedural designs for drinking water systems and in controlling exposure to Legionella spp. and similar pathogens.
- 53Scheikl, U.; Sommer, R.; Kirschner, A.; Rameder, A.; Schrammel, B.; Zweimuller, I.; Wesner, W.; Hinker, M.; Walochnik, J. Free-living amoebae (FLA) co-occurring with legionellae in industrial waters. Eur. J. Protistol.IF 2.9SCIEJCI 0.69Q3生物学2区2014, 50 (4), 422– 429, DOI: 10.1016/j.ejop.2014.04.002 53https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A280%3ADC%252BC2cblvVyhsg%253D%253D&md5=0e75f9aa592e6ae6af5a17256640cd42Free-living amoebae (FLA) co-occurring with legionellae in industrial watersScheikl Ute; Sommer Regina; Kirschner Alexander; Rameder Alexandra; Schrammel Barbara; Zweimuller Irene; Wesner Wolfgang; Hinker Manfred; Walochnik JuliaEuropean journal of protistology (2014), 50 (4), 422-9 ISSN:.Legionella pneumophila is known as the causative agent of Legionnaires' disease and free-living amoebae (FLA) can serve as vehicles for legionellae. The aim of this study was to screen industrial waters for the occurrence of FLA and their co-occurrence with legionellae. A total of 201 water samples, including 129 cooling waters and 72 process waters, and 30 cooling lubricants were included in the study. Treated waters were screened periodically, pre and post treatment. Altogether, 72.6% of the water samples were positive for FLA, acanthamoebae being most prevalent (in 23.9% of the samples) followed by Vermamoeba vermiformis (19.4%). Only one cooling lubricant was positive (Acanthamoeba genotype T4). Legionella spp. were detected in 34.8% of the water samples and in 15% in high concentrations (>1000 CFU/100 ml). Altogether, 81.4% of the Legionella-positive samples were positive for FLA by standard methods. By applying a highly sensitive nested PCR to a representative set of random samples it was revealed that Legionella spp. always co-occurred with Acanthamoeba spp. Although the addition of disinfectants did influence amoebal density and diversity, treated waters showed no difference concerning FLA in the interphases of disinfection. It appears that FLA can re-colonize treated waters within a short period of time.
- 54Caicedo, C.; Rosenwinkel, K.-H.; Exner, M.; Verstraete, W.; Suchenwirth, R.; Hartemann, P.; Nogueira, R. Legionella occurrence in municipal and industrial wastewater treatment plants and risks of reclaimed wastewater reuse: Review. Water Res.IF 12.8SCIEJCI 2.15Q1环境科学与生态学1区Top2019, 149, 21– 34, DOI: 10.1016/j.watres.2018.10.080 54https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BC1cXitFyhurbF&md5=7fbe53b1bb2a7053e7504a0499f2ccabLegionella occurrence in municipal and industrial wastewater treatment plants and risks of reclaimed wastewater reuse: ReviewCaicedo, C.; Rosenwinkel, K.-H.; Exner, M.; Verstraete, W.; Suchenwirth, R.; Hartemann, P.; Nogueira, R.Water Research (2019), 149 (), 21-34CODEN: WATRAG; ISSN:0043-1354. (Elsevier Ltd.)Wastewater treatment plants (WWTPs) have been identified as confirmed but until today underestimated sources of Legionella, playing an important role in local and community cases and outbreaks of Legionnaires' disease. In general, aerobic biol. systems provide an optimum environment for the growth of Legionella due to high org. nitrogen and oxygen concns., ideal temps. and the presence of protozoa. However, few studies have investigated the occurrence of Legionella in WWTPs, and many questions in regards to the interacting factors that promote the proliferation and persistence of Legionella in these treatment systems are still unanswered. This crit. review summarizes the current knowledge about Legionella in municipal and industrial WWTPs, the conditions that might support their growth, as well as control strategies that have been applied. Furthermore, an overview of current quantification methods, guidelines and health risks assocd. with Legionella in reclaimed wastewater is also discussed in depth. A better understanding of the conditions promoting the occurrence of Legionella in WWTPs will contribute to the development of improved wastewater treatment technologies and/or innovative mitigation approaches to minimize future Legionella outbreaks.
- 55Gerrity, D.; Arnold, M.; Dickenson, E.; Moser, D.; Sackett, J. D.; Wert, E. C. Microbial community characterization of ozone-biofiltration systems in drinking water and potable reuse applications. Water Res.IF 12.8SCIEJCI 2.15Q1环境科学与生态学1区Top2018, 135, 207– 219, DOI: 10.1016/j.watres.2018.02.023 There is no corresponding record for this reference.
- 56Zhang, L.; Graham, N.; Li, G.; Yu, W. Divergent accumulation of membrane biofouling by slight elevation of nitrogen and phosphorus in drinking water treatment: Performances and mechanisms. Water Res.IF 12.8SCIEJCI 2.15Q1环境科学与生态学1区Top2022, 222, 118898, DOI: 10.1016/j.watres.2022.118898 There is no corresponding record for this reference.
- 57Desmond, P.; Huisman, K. T.; Sanawar, H.; Farhat, N. M.; Traber, J.; Fridjonsson, E. O.; Johns, M. L.; Flemming, H.-C.; Picioreanu, C.; Vrouwenvelder, J. S. Controlling the hydraulic resistance of membrane biofilms by engineering biofilm physical structure. Water Res.IF 12.8SCIEJCI 2.15Q1环境科学与生态学1区Top2022, 210, 118031, DOI: 10.1016/j.watres.2021.118031 57https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BB38XksFKitQ%253D%253D&md5=ee3251a57598a194d198d95270b37ae8Controlling the hydraulic resistance of membrane biofilms by engineering biofilm physical structureDesmond, Peter; Huisman, Kees Theo; Sanawar, Huma; Farhat, Nadia M.; Traber, Jacqueline; Fridjonsson, Einar O.; Johns, Michael L.; Flemming, Hans-Curt; Picioreanu, Cristian; Vrouwenvelder, Johannes S.Water Research (2022), 210 (), 118031CODEN: WATRAG; ISSN:0043-1354. (Elsevier Ltd.)A review. The application of membrane technol. for water treatment and reuse is hampered by the development of a microbial biofilm. Biofilm growth in micro-and ultrafiltration (MF/UF) membrane modules, on both the membrane surface and feed spacer, can form a secondary membrane and exert resistance to permeation and crossflow, increasing energy demand and decreasing permeate quantity and quality. In recent years, exhaustive efforts were made to understand the chem., structural and hydraulic characteristics of membrane biofilms. In this , we critically assess which specific structural features of membrane biofilms exert resistance to forced water passage in MF/UF membranes systems applied to water and wastewater treatment, and how biofilm phys. structure can be engineered by process operation to impose less hydraulic resistance ("below-the-pain threshold"). Counter-intuitively, biofilms with greater thickness do not always cause a higher hydraulic resistance than thinner biofilms. Dense biofilms, however, had consistently higher hydraulic resistances compared to less dense biofilms. The mechanism by which d. exerts hydraulic resistance is reported in the literature to be dependant on the biofilms' internal packing structure and EPS chem. compd. (e.g., porosity, polymer concn.). Current reports of internal porosity in membrane biofilms are not supported by adequate exptl. evidence or by a reliable methodol., limiting a unified understanding of biofilm internal structure. Identifying the dependency of hydraulic resistance on biofilm d. invites efforts to control the hydraulic resistance of membrane biofilms by engineering internal biofilm structure. Regulation of biofilm internal structure is possible by alteration of key determinants such as feed water nutrient compd./concn., hydraulic shear stress and resistance and can engineer biofilm structural development to decrease d. and therein hydraulic resistance. Future efforts should seek to det. the extent to which the concept of "biofilm engineering" can be extended to other biofilm parameters such as mech. stability and the implication for biofilm control/removal in engineered water systems (e.g., pipelines and/or, cooling towers) susceptible to biofouling.
- 58Abada, B.; Safarik, J.; Ishida, K. P.; Chellam, S. Surface characterization of end-of-life reverse osmosis membranes from a full-scale advanced water reuse facility: Combined role of bioorganic materials and silicon on chemically irreversible fouling. J. Membr. Sci.IF 9.5SCIEJCI 1.85Q1工程技术1区Top2022, 653, 120511, DOI: 10.1016/j.memsci.2022.120511 58https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BB38XpsVygtLg%253D&md5=451543b823a01355c995ea63b3ba2462Surface characterization of end-of-life reverse osmosis membranes from a full-scale advanced water reuse facility: Combined role of bioorganic materials and silicon on chemically irreversible foulingAbada, Bilal; Safarik, Jana; Ishida, Kenneth P.; Chellam, ShankararamanJournal of Membrane Science (2022), 653 (), 120511CODEN: JMESDO; ISSN:0376-7388. (Elsevier B.V.)Eight-year-old end-of-life reverse osmosis (RO) membranes from all three stages of a full-scale plant from the world's largest potable reuse facility were comprehensively characterized to discern the role of the co-existing foulants on performance decline and recovery by chem. cleaning. XPS and energy dispersive X-ray spectra detected surficial silica foulants on all stages. High-resoln. XPS and IR spectra evidenced siloxanes among other forms of silicon foulants, which was confirmed by gas chromatog.-mass spectrometry as cyclosiloxanes. Addnl., culturable bacteria were recovered, and other bioorg. foulants were identified by colorimetry, microscopy, and spectroscopy. Higher amts. of bioorg. foulants were measured in the first two stages, whereas silica fouling was more significant in the first- and third-stage elements. Chem. cleaning with either sodium tripolyphosphate - sodium dodecylbenzenesulfonic acid mixt., sodium dodecyl sulfate - sodium hydroxide mixt., or hydrochloric acid did not completely restore membrane permeability demonstrating the need for membrane replacement. Siliceous foulants were most intractable to all chem. cleaning methods evaluated (including sodium hydroxide) and were the dominant cause of chem.-irreversible fouling leading to the membranes' end-of-life. Our results suggest that incorporating silicon pretreatment could improve RO performance and extend membrane life span during municipal potable reuse.
- 59Ivleva, N. P.; Wagner, M.; Horn, H.; Niessner, R.; Haisch, C. Towards a nondestructive chemical characterization of biofilm matrix by Raman microscopy. Anal. Bioanal. Chem.IF 4.3SCIEJCI 0.93Q1化学2区2009, 393 (1), 197– 206, DOI: 10.1007/s00216-008-2470-5 There is no corresponding record for this reference.
- 60Laue, H.; Schenk, A.; Li, H.; Lambertsen, L.; Neu, T. R.; Molin, S.; Ullrich, M. S. Contribution of alginate and levan production to biofilm formation by Pseudomonas syringae. Microbiolology 2006, 152 (10), 2909– 2918, DOI: 10.1099/mic.0.28875-0 There is no corresponding record for this reference.
Supporting Information
Supporting Information
ARTICLE SECTIONSThe Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.est.3c10429.
The Supporting Information includes 4 figures and 3 tables, which supplement the results in the manuscript. These comprise the following: schematic diagram of membrane filtration system (Figure S1), FT-ICR mass spectra of influent DOM in membrane filtration systems (Figure S2), XPS full spectra of biofilms (Figure S3), variation in permeate flux of membrane filtration systems in the course of each experiment (Figure S4), principal water quality parameters of surface water (Table S1), area percent of XPS spectral peaks (Table S2), and biofilm surface texture of roughness data set (Table S3) (PDF)
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