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Dissociation-dependent kinetics and distinct pathways for direct photolysis and •OH/SO4•− radical dominated photodegradation of ionizable antiviral drugs in aquatic systems 可离子化抗病毒药物在水生系统中直接光解和 OH/SO4- 自由基主导光降解的解离依赖动力学和不同途径
IF 11.4 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2025-03-09 DOI: 10.1016/j.watres.2025.123452
Nannan Cui , Linke Ge , Crispin Halsall , Junfeng Niu , Jinshuai Zheng , Peng Zhang
Advanced oxidation processes (AOPs), such as UV, UV/H2O2 and UV/persulfate, are widely used to remove emerging organic contaminants from wastewater streams. However, knowledge on chemical degradation pathways, reaction kinetics as well as formation and toxicity of key degradates is limited. We investigated the direct photolysis and •OH/SO4•− dominated kinetics, intermediates and toxicity evolution of three ionizable antiviral drugs (ATVs): tenofovir (TFV), didanosine (DDI), and nevirapine (NVP). Their transformation kinetics were found to depend on the dominant protonated states. Under UV–Vis irradiation (λ > 290 nm), TFV and DDI photolyzed the fastest in the cationic forms (H2TFV+ and H2DDI+), whereas NVP exhibited the fastest photodegradation in the anionic forms (NVP). The anionic forms (TFV and NVP) demonstrated the highest reactivities towards •OH in most cases, while the cationic forms (H2DDI+ and H2NVP+) reacted the fastest with SO4•− for most of the ATVs. The dissociation-dependent kinetics can be attributed to the discrepancies in deprotonation degrees, quantum yields, electron densities and coulombic repulsion with SO4•− in their dissociated forms. Based on the key product identification via HPLC-MS/MS, the pathways involved hydroxylation, dehydroxylation, oxidation, reduction, cyclopropyl cleavage, C-N breaking, elimination, cyclization and deamidation reactions, which can be prioritized based on the specific compound and the photochemical process. Furthermore, a bioassay showed the photomodified toxicity of the ATVs to Vibrio fischeri (bioluminescent bacteria) during the three processes, which was also demonstrated by ECOSAR model assessment. Nearly half of the chemical intermediates were demonstrably more toxic than their respective parent ATVs. These results provide new insights into understanding the persistence, fate and hazards associated with applying the UV-assisted AOPs to treat wastewater containing ATVs.
{"title":"Dissociation-dependent kinetics and distinct pathways for direct photolysis and •OH/SO4•− radical dominated photodegradation of ionizable antiviral drugs in aquatic systems","authors":"Nannan Cui ,&nbsp;Linke Ge ,&nbsp;Crispin Halsall ,&nbsp;Junfeng Niu ,&nbsp;Jinshuai Zheng ,&nbsp;Peng Zhang","doi":"10.1016/j.watres.2025.123452","DOIUrl":"10.1016/j.watres.2025.123452","url":null,"abstract":"<div><div>Advanced oxidation processes (AOPs), such as UV, UV/H<sub>2</sub>O<sub>2</sub> and UV/persulfate, are widely used to remove emerging organic contaminants from wastewater streams. However, knowledge on chemical degradation pathways, reaction kinetics as well as formation and toxicity of key degradates is limited. We investigated the direct photolysis and •OH/SO<sub>4</sub><sup>•−</sup> dominated kinetics, intermediates and toxicity evolution of three ionizable antiviral drugs (ATVs): tenofovir (TFV), didanosine (DDI), and nevirapine (NVP). Their transformation kinetics were found to depend on the dominant protonated states. Under UV–Vis irradiation (<em>λ</em> &gt; 290 nm), TFV and DDI photolyzed the fastest in the cationic forms (H<sub>2</sub>TFV<sup>+</sup> and H<sub>2</sub>DDI<sup>+</sup>), whereas NVP exhibited the fastest photodegradation in the anionic forms (NVP<sup>−</sup>). The anionic forms (TFV<sup>−</sup> and NVP<sup>−</sup>) demonstrated the highest reactivities towards •OH in most cases, while the cationic forms (H<sub>2</sub>DDI<sup>+</sup> and H<sub>2</sub>NVP<sup>+</sup>) reacted the fastest with SO<sub>4</sub><sup>•−</sup> for most of the ATVs. The dissociation-dependent kinetics can be attributed to the discrepancies in deprotonation degrees, quantum yields, electron densities and coulombic repulsion with SO<sub>4</sub><sup>•−</sup> in their dissociated forms. Based on the key product identification via HPLC-MS/MS, the pathways involved hydroxylation, dehydroxylation, oxidation, reduction, cyclopropyl cleavage, C-N breaking, elimination, cyclization and deamidation reactions, which can be prioritized based on the specific compound and the photochemical process. Furthermore, a bioassay showed the photomodified toxicity of the ATVs to <em>Vibrio fischeri</em> (bioluminescent bacteria) during the three processes, which was also demonstrated by ECOSAR model assessment. Nearly half of the chemical intermediates were demonstrably more toxic than their respective parent ATVs. These results provide new insights into understanding the persistence, fate and hazards associated with applying the UV-assisted AOPs to treat wastewater containing ATVs.</div></div>","PeriodicalId":443,"journal":{"name":"Water Research","volume":"279 ","pages":"Article 123452"},"PeriodicalIF":11.4,"publicationDate":"2025-03-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143576197","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Making waves: Pioneering a nanoconfinement platform with mesoporous silica for sustainable water management and environmental applications 掀起波澜:利用介孔二氧化硅开创用于可持续水管理和环境应用的纳米融合平台
IF 11.4 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2025-03-08 DOI: 10.1016/j.watres.2025.123460
Haklae Lee , Han Fu , Kimberly A. Gray
Nanomaterials applied in industrial processes and environmental fields usually demand immobilization and recovery strategies that often result in functionality loss and added operational costs. Nanoconfinement, the spatial restriction of nano-sized particles within a larger porous substrate, not only can address critical challenges and sustainability concerns in environmental nanotechnology but also offers unique opportunities otherwise inaccessible by unconfined, bulk-phase nanomaterials. In this perspective, we propose mesoporous silica (mSiO2) as an innovative framework for spatially confining metal nanoparticles in a well-controlled manner, offering an effective nanoconfinement engineering strategy for sustainable water management and environmental applications. We first summarize the current understanding of nanoconfinement effects and briefly review previous approaches to the fabrication of engineered nanoconfinement materials. We then present a layer-by-layer engineering strategy to confine various metal nanoparticles within multi-shelled mSiO2 structures, exploring their unique nanoconfinement features and potential environmental applications, e.g. tandem catalysis, surface-enhanced Raman scattering (SERS) sensor, and visible-light-driven water treatment. Finally, we discuss challenges in studying nanoconfinement effects and outline future research directions to advance sustainable innovation. Opportunities for practical implementation exist at the intersection of fundamental studies and engineering disciplines, emphasizing the need for parallel efforts to establish system characterization standards and enable effective technological integration at scale.
{"title":"Making waves: Pioneering a nanoconfinement platform with mesoporous silica for sustainable water management and environmental applications","authors":"Haklae Lee ,&nbsp;Han Fu ,&nbsp;Kimberly A. Gray","doi":"10.1016/j.watres.2025.123460","DOIUrl":"10.1016/j.watres.2025.123460","url":null,"abstract":"<div><div>Nanomaterials applied in industrial processes and environmental fields usually demand immobilization and recovery strategies that often result in functionality loss and added operational costs. Nanoconfinement, the spatial restriction of nano-sized particles within a larger porous substrate, not only can address critical challenges and sustainability concerns in environmental nanotechnology but also offers unique opportunities otherwise inaccessible by unconfined, bulk-phase nanomaterials. In this perspective, we propose mesoporous silica (mSiO<sub>2</sub>) as an innovative framework for spatially confining metal nanoparticles in a well-controlled manner, offering an effective nanoconfinement engineering strategy for sustainable water management and environmental applications. We first summarize the current understanding of nanoconfinement effects and briefly review previous approaches to the fabrication of engineered nanoconfinement materials. We then present a layer-by-layer engineering strategy to confine various metal nanoparticles within multi-shelled mSiO<sub>2</sub> structures, exploring their unique nanoconfinement features and potential environmental applications, e.g. tandem catalysis, surface-enhanced Raman scattering (SERS) sensor, and visible-light-driven water treatment. Finally, we discuss challenges in studying nanoconfinement effects and outline future research directions to advance sustainable innovation. Opportunities for practical implementation exist at the intersection of fundamental studies and engineering disciplines, emphasizing the need for parallel efforts to establish system characterization standards and enable effective technological integration at scale.</div></div>","PeriodicalId":443,"journal":{"name":"Water Research","volume":"280 ","pages":"Article 123460"},"PeriodicalIF":11.4,"publicationDate":"2025-03-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143576219","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Uncharacterized members of the phylum Rozellomycota dominate the fungal community of a full-scale slow sand filter for drinking water production.
IF 11.4 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2025-03-08 DOI: 10.1016/j.watres.2025.123447
Tage Rosenqvist , Sandy Chan , Catherine J. Paul
Slow sand filters (SSFs) for drinking water production are habitats for diverse microbes from multiple domains of life, which are integral to the ability of SSFs to purify water. While cultivation-independent analyses of the prokaryotic communities of SSFs have provided valuable insights, little attention has been paid to fungi inhabiting SSFs. This study characterized the fungal communities in the sand biofilm of one established, one inoculated and one non-inoculated SSF. The removal of the top-layer of sand (“scraping”) allowed fungal communities in the top and subsurface layers of sand to be analyzed using amplicon sequencing of the ITS2 region of fungal rRNA genes.
The top layers of SSF sand contained fungal communities dominated by phylum Ascomycota (43.5–75.6 %). After scraping, high abundances (>70 %) of phylum Rozellomycota were revealed in the established filter. These fungi were also detected in an inoculated filter, but not in a non-inoculated filter, suggesting potential dispersal to new filters by inoculation. The diverse Rozellomycota sequences potentially represented 6 different order-level clades, with most being related to previously observed Branch03 Rozellomycota. Their roles in SSF function are unknown but may be related to the removal of indicator bacteria as this phylum includes potential parasites of grazing eukaryotes. Fungi known to constitute microbial risk or contribute to micropollutant biodegradation were in low abundance and only sporadically detected. Lifestyle traits could be predicted for 61.8 % of fungi in the SSF biofilm; most of these were saprotrophic microfungi or yeasts.
This study presents an overview of the composition of fungal communities in full-scale SSF, and their potential interactions with water quality. It also highlights the need for more knowledge regarding the ecology of “dark matter”-fungi, such as Rozellomycota, and presents an accessible and societally relevant environment for future research of these microbes.
{"title":"Uncharacterized members of the phylum Rozellomycota dominate the fungal community of a full-scale slow sand filter for drinking water production.","authors":"Tage Rosenqvist ,&nbsp;Sandy Chan ,&nbsp;Catherine J. Paul","doi":"10.1016/j.watres.2025.123447","DOIUrl":"10.1016/j.watres.2025.123447","url":null,"abstract":"<div><div>Slow sand filters (SSFs) for drinking water production are habitats for diverse microbes from multiple domains of life, which are integral to the ability of SSFs to purify water. While cultivation-independent analyses of the prokaryotic communities of SSFs have provided valuable insights, little attention has been paid to fungi inhabiting SSFs. This study characterized the fungal communities in the sand biofilm of one established, one inoculated and one non-inoculated SSF. The removal of the top-layer of sand (“scraping”) allowed fungal communities in the top and subsurface layers of sand to be analyzed using amplicon sequencing of the ITS2 region of fungal rRNA genes.</div><div>The top layers of SSF sand contained fungal communities dominated by phylum <em>Ascomycota</em> (43.5–75.6 %). After scraping, high abundances (&gt;70 %) of phylum <em>Rozellomycota</em> were revealed in the established filter. These fungi were also detected in an inoculated filter, but not in a non-inoculated filter, suggesting potential dispersal to new filters by inoculation. The diverse <em>Rozellomycota</em> sequences potentially represented 6 different order-level clades, with most being related to previously observed Branch03 <em>Rozellomycota</em>. Their roles in SSF function are unknown but may be related to the removal of indicator bacteria as this phylum includes potential parasites of grazing eukaryotes. Fungi known to constitute microbial risk or contribute to micropollutant biodegradation were in low abundance and only sporadically detected. Lifestyle traits could be predicted for 61.8 % of fungi in the SSF biofilm; most of these were saprotrophic microfungi or yeasts.</div><div>This study presents an overview of the composition of fungal communities in full-scale SSF, and their potential interactions with water quality. It also highlights the need for more knowledge regarding the ecology of “dark matter”-fungi, such as <em>Rozellomycota</em>, and presents an accessible and societally relevant environment for future research of these microbes.</div></div>","PeriodicalId":443,"journal":{"name":"Water Research","volume":"279 ","pages":"Article 123447"},"PeriodicalIF":11.4,"publicationDate":"2025-03-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143576220","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Viscosity is a nonnegligible factor in the waste activated sludge fermentation: Taking hyaluronan as an example
IF 11.4 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2025-03-08 DOI: 10.1016/j.watres.2025.123465
Yan-Lin Hu , Kun Dai , Qing-Ting Wang , Chen-Yuan Zhou , Xing-Chen Huang , Xiao-Fei Yang , He-Liang Pang , Raymond Jianxiong Zeng , Fang Zhang
The waste activated sludge (WAS) exhibits typical viscoelasticity due to the presence of viscous and gelling organics in extracellular polymeric substances (EPS). However, the positive role of reducing viscosity in WAS fermentation by degrading viscous polysaccharides has been historically overlooked. This work demonstrates the occurrence of viscous hyaluronan-like polysaccharides in the WAS for the first time. Approximately 6.8 % of bacteria, such as Zoogloea (1.0 %), were identified as the potential producers. The viscosity of hyaluronan could be significantly reduced by 99 % within 1 hour by the oriented hyaluronan-degrading consortium (HDC), and a reduction of 20 % was also observed for WAS after 24 h. This resulted in a 18 % improvement in methane production and a 35 % improvement in the maximum production rate in WAS fermentation. The conversion of viscous hyaluronan was mainly through the hyaluronan lyase (EC 4.2.2.1) dependent pathway. An unfamiliar genus of Paludibacter (9.6 %) was identified as a key bacterium, responsible for excreting five extracellular enzymes of EC 4.2.2.1, EC 3.2.1.35, EC 3.2.1.31, EC 3.2.1.52, and EC 3.2.1.180. Consequently, this study has elucidated reducing viscosity as a substantial factor in WAS fermentation by the oriented HDC, thus providing a novel paradigm to enhance methane production.
{"title":"Viscosity is a nonnegligible factor in the waste activated sludge fermentation: Taking hyaluronan as an example","authors":"Yan-Lin Hu ,&nbsp;Kun Dai ,&nbsp;Qing-Ting Wang ,&nbsp;Chen-Yuan Zhou ,&nbsp;Xing-Chen Huang ,&nbsp;Xiao-Fei Yang ,&nbsp;He-Liang Pang ,&nbsp;Raymond Jianxiong Zeng ,&nbsp;Fang Zhang","doi":"10.1016/j.watres.2025.123465","DOIUrl":"10.1016/j.watres.2025.123465","url":null,"abstract":"<div><div>The waste activated sludge (WAS) exhibits typical viscoelasticity due to the presence of viscous and gelling organics in extracellular polymeric substances (EPS). However, the positive role of reducing viscosity in WAS fermentation by degrading viscous polysaccharides has been historically overlooked. This work demonstrates the occurrence of viscous hyaluronan-like polysaccharides in the WAS for the first time. Approximately 6.8 % of bacteria, such as <em>Zoogloea</em> (1.0 %), were identified as the potential producers. The viscosity of hyaluronan could be significantly reduced by 99 % within 1 hour by the oriented hyaluronan-degrading consortium (HDC), and a reduction of 20 % was also observed for WAS after 24 h. This resulted in a 18 % improvement in methane production and a 35 % improvement in the maximum production rate in WAS fermentation. The conversion of viscous hyaluronan was mainly through the hyaluronan lyase (EC 4.2.2.1) dependent pathway. An unfamiliar genus of <em>Paludibacter</em> (9.6 %) was identified as a key bacterium, responsible for excreting five extracellular enzymes of EC 4.2.2.1, EC 3.2.1.35, EC 3.2.1.31, EC 3.2.1.52, and EC 3.2.1.180. Consequently, this study has elucidated reducing viscosity as a substantial factor in WAS fermentation by the oriented HDC, thus providing a novel paradigm to enhance methane production.</div></div>","PeriodicalId":443,"journal":{"name":"Water Research","volume":"279 ","pages":"Article 123465"},"PeriodicalIF":11.4,"publicationDate":"2025-03-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143576331","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Heatwave enhance the adaptability of Chlorella pyrenoidosa to zinc oxide nanoparticles: Regulation of interfacial interactions and metabolic mechanisms
IF 11.4 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2025-03-08 DOI: 10.1016/j.watres.2025.123466
Keyi Huang , Hui Zeng , Qixing Zhou
Wide application of zinc oxide nanoparticles (ZnO NPs) and increasing frequency of heatwaves (HWs) have posed a great threat to freshwater ecosystems, while phytotoxicity of ZnO NPs mediated by HWs remains unclear. This study aims to link the physiological responses, bio-nano interactions, and metabolic mechanisms of Chlorella pyrenoidosa with ZnO NPs under heat stress. Results demonstrated a temperature-dependent growth inhibition against ZnO NPs, with a higher reduction of growth rate at 24 °C than 28 °C. Accompanied with lower reactive oxidative stress and cell damage at 28 °C, our results indicated that HW could enhance the adaptability of C. pyrenoidosa to ZnO NPs stress. Furthermore, HW induced the variation of algal surface properties, altered interfacial interactions in the bio-nano system, and decreased cellular Zn uptake. Metabolomics analysis supported the temperature-dependent influences of ZnO NPs on C. pyrenoidosa. The phytotoxicity of ZnO NPs was associated with the disturbance of amino acids, fatty acids, and energy metabolic processes, which were mitigated under HW condition, enhancing the responsiveness of algae to the adverse effects. These results emphasize the importance of taking the impacts of HWs into account when evaluating the environmental risks of ZnO NPs.
{"title":"Heatwave enhance the adaptability of Chlorella pyrenoidosa to zinc oxide nanoparticles: Regulation of interfacial interactions and metabolic mechanisms","authors":"Keyi Huang ,&nbsp;Hui Zeng ,&nbsp;Qixing Zhou","doi":"10.1016/j.watres.2025.123466","DOIUrl":"10.1016/j.watres.2025.123466","url":null,"abstract":"<div><div>Wide application of zinc oxide nanoparticles (ZnO NPs) and increasing frequency of heatwaves (HWs) have posed a great threat to freshwater ecosystems, while phytotoxicity of ZnO NPs mediated by HWs remains unclear. This study aims to link the physiological responses, bio-nano interactions, and metabolic mechanisms of <em>Chlorella pyrenoidosa</em> with ZnO NPs under heat stress. Results demonstrated a temperature-dependent growth inhibition against ZnO NPs, with a higher reduction of growth rate at 24 °C than 28 °C. Accompanied with lower reactive oxidative stress and cell damage at 28 °C, our results indicated that HW could enhance the adaptability of <em>C. pyrenoidosa</em> to ZnO NPs stress. Furthermore, HW induced the variation of algal surface properties, altered interfacial interactions in the bio-nano system, and decreased cellular Zn uptake. Metabolomics analysis supported the temperature-dependent influences of ZnO NPs on <em>C. pyrenoidosa</em>. The phytotoxicity of ZnO NPs was associated with the disturbance of amino acids, fatty acids, and energy metabolic processes, which were mitigated under HW condition, enhancing the responsiveness of algae to the adverse effects. These results emphasize the importance of taking the impacts of HWs into account when evaluating the environmental risks of ZnO NPs.</div></div>","PeriodicalId":443,"journal":{"name":"Water Research","volume":"279 ","pages":"Article 123466"},"PeriodicalIF":11.4,"publicationDate":"2025-03-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143576216","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Green and efficient disinfection of antibiotic-resistant bacteria via PI/H2O2 homogeneous system
IF 11.4 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2025-03-08 DOI: 10.1016/j.watres.2025.123468
Boaiqi Zhang , Zhengmao Li , Fuyang Liu , Xiangwei Zhang , Yanghui Hou , Meiping Tong
The proliferation and spread of antibiotic-resistant bacteria (ARB) significantly threaten human health and ecosystem. Periodate (PI) based advanced oxidation process has potentials for water purification but is limited by complex activators or activation process. Herein, we demonstrated that H2O2 could be used to activate PI, achieving efficient ARB disinfection performance. Particularly, we found that the PI/H2O2 system (0.1 mM for both oxidants) could inactivate ARB (Escherichia coli) within 35 min. The intracellular defense system could be attacked by HO· radicals generated in the disinfection system, resulting in the inactivation of ARB. Antibiotic resistance genes (ARGs) released with the lysis of cell membrane could be further degraded by HO· radicals. Moreover, we found that the PI/H2O2 system was effective to inactivate ARB in a broad range of ionic strengths, with coexisting common ions and humic acid, as well as in four typical actual water bodies. The PI/H2O2 system could also efficiently disinfect other types of bacteria and degrade typical organic contaminants. In addition, under sunlight irradiation, the ARB inactivation performance of the PI/H2O2 system could be greatly improved. This study provided a practical and efficient way for decontaminating ARB/ARGs-polluted water.
{"title":"Green and efficient disinfection of antibiotic-resistant bacteria via PI/H2O2 homogeneous system","authors":"Boaiqi Zhang ,&nbsp;Zhengmao Li ,&nbsp;Fuyang Liu ,&nbsp;Xiangwei Zhang ,&nbsp;Yanghui Hou ,&nbsp;Meiping Tong","doi":"10.1016/j.watres.2025.123468","DOIUrl":"10.1016/j.watres.2025.123468","url":null,"abstract":"<div><div>The proliferation and spread of antibiotic-resistant bacteria (ARB) significantly threaten human health and ecosystem. Periodate (PI) based advanced oxidation process has potentials for water purification but is limited by complex activators or activation process. Herein, we demonstrated that H<sub>2</sub>O<sub>2</sub> could be used to activate PI, achieving efficient ARB disinfection performance. Particularly, we found that the PI/H<sub>2</sub>O<sub>2</sub> system (0.1 mM for both oxidants) could inactivate ARB (<em>Escherichia coli</em>) within 35 min. The intracellular defense system could be attacked by HO<sup>·</sup> radicals generated in the disinfection system, resulting in the inactivation of ARB. Antibiotic resistance genes (ARGs) released with the lysis of cell membrane could be further degraded by HO<sup>·</sup> radicals. Moreover, we found that the PI/H<sub>2</sub>O<sub>2</sub> system was effective to inactivate ARB in a broad range of ionic strengths, with coexisting common ions and humic acid, as well as in four typical actual water bodies. The PI/H<sub>2</sub>O<sub>2</sub> system could also efficiently disinfect other types of bacteria and degrade typical organic contaminants. In addition, under sunlight irradiation, the ARB inactivation performance of the PI/H<sub>2</sub>O<sub>2</sub> system could be greatly improved. This study provided a practical and efficient way for decontaminating ARB/ARGs-polluted water.</div></div>","PeriodicalId":443,"journal":{"name":"Water Research","volume":"280 ","pages":"Article 123468"},"PeriodicalIF":11.4,"publicationDate":"2025-03-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143576217","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
A clustering approach based on high-resolution ecological vulnerability index reveals spatial patterns of per- and polyfluoroalkyl substances pollution in lakes on the Tibetan Plateau 基于高分辨率生态脆弱性指数的聚类方法揭示了青藏高原湖泊全氟和多氟烷基物质污染的空间模式
IF 11.4 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2025-03-08 DOI: 10.1016/j.watres.2025.123461
Xu Han , Baozhu Pan , Zhile Pan , Nan Xu , Jiang Wu , Weiling Sun , Bowen Hou , Yanran Dong
Per- and polyfluoroalkyl substances (PFAS) are persistent organic pollutants (POPs) with toxicity, chemical stability, and long-range transport potential. The transport and accumulation mechanisms of PFAS in specific or typical lakes have been reported. In the wake of global PFAS pollution, it is more important to unravel the distribution patterns of PFAS across larger-scale, multi-lake systems. However, traditional lake classification methods are often overly simplistic and inflexible to adapt to large lake systems with complex ecological characteristics. Here, an improved ecological vulnerability index (EVI) was introduced and applied for the first time to classify lakes in a regional, multi-lake study of PFAS pollution. We evaluated the effectiveness of EVI that integrated multi-dimensional environmental factors in revealing PFAS distribution in 12 lakes on the Tibetan Plateau. The results showed that the composition, concentration, and diversity of PFAS in water and sediment samples significantly differed between high-vulnerability lakes (HVL) and low-vulnerability lakes (LVL) clustered by EVI. The linear regression of PFAS concentration and diversity on EVI was most pronounced at the 1-km buffer zone scale compared to larger scales. EVI was strongly associated with PFAS concentration and diversity in HVL dominated by natural factors, and these associations were weakened in LVL with prevalent human interference. Our findings indicate the greater potential of EVI to predict the spatial patterns of PFAS in lakes at smaller scales and across regions with comparable dominance of natural factors. The proposed clustering approach is adaptable, as the indicators and weights in the EVI system can be adjusted based on regional ecological characteristics. This study provides a tool for unveiling the distribution patterns of PFAS and their driving mechanisms in complex lake environments.
{"title":"A clustering approach based on high-resolution ecological vulnerability index reveals spatial patterns of per- and polyfluoroalkyl substances pollution in lakes on the Tibetan Plateau","authors":"Xu Han ,&nbsp;Baozhu Pan ,&nbsp;Zhile Pan ,&nbsp;Nan Xu ,&nbsp;Jiang Wu ,&nbsp;Weiling Sun ,&nbsp;Bowen Hou ,&nbsp;Yanran Dong","doi":"10.1016/j.watres.2025.123461","DOIUrl":"10.1016/j.watres.2025.123461","url":null,"abstract":"<div><div>Per- and polyfluoroalkyl substances (PFAS) are persistent organic pollutants (POPs) with toxicity, chemical stability, and long-range transport potential. The transport and accumulation mechanisms of PFAS in specific or typical lakes have been reported. In the wake of global PFAS pollution, it is more important to unravel the distribution patterns of PFAS across larger-scale, multi-lake systems. However, traditional lake classification methods are often overly simplistic and inflexible to adapt to large lake systems with complex ecological characteristics. Here, an improved ecological vulnerability index (EVI) was introduced and applied for the first time to classify lakes in a regional, multi-lake study of PFAS pollution. We evaluated the effectiveness of EVI that integrated multi-dimensional environmental factors in revealing PFAS distribution in 12 lakes on the Tibetan Plateau. The results showed that the composition, concentration, and diversity of PFAS in water and sediment samples significantly differed between high-vulnerability lakes (HVL) and low-vulnerability lakes (LVL) clustered by EVI. The linear regression of PFAS concentration and diversity on EVI was most pronounced at the 1-km buffer zone scale compared to larger scales. EVI was strongly associated with PFAS concentration and diversity in HVL dominated by natural factors, and these associations were weakened in LVL with prevalent human interference. Our findings indicate the greater potential of EVI to predict the spatial patterns of PFAS in lakes at smaller scales and across regions with comparable dominance of natural factors. The proposed clustering approach is adaptable, as the indicators and weights in the EVI system can be adjusted based on regional ecological characteristics. This study provides a tool for unveiling the distribution patterns of PFAS and their driving mechanisms in complex lake environments.</div></div>","PeriodicalId":443,"journal":{"name":"Water Research","volume":"279 ","pages":"Article 123461"},"PeriodicalIF":11.4,"publicationDate":"2025-03-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143576329","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
A hollow fiber supported ionic liquid membrane contactor for continuous extraction of lithium from high magnesium/lithium ratio brine
IF 11.4 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2025-03-07 DOI: 10.1016/j.watres.2025.123451
Bo Dong , Junyuan Hua , Jintao He , Jiahui Du , Jian Xiao , Jianxin Li
High-efficiency lithium (Li+) extraction from a salt-lake brine with a low Li concentration and a high Mg/Li mass ratio poses a great challenge owing to the great physical and chemical similarities between Mg2+ and Li+. In this study, a hollow fiber (HF) membrane with an inside diameter of 0.872 mm and an outside diameter of 1.228 mm was fabricated using nonsolvent induce phase separation method with 14-crown-4 ether functionalized polyimide (14C4PI) as a polymer matrix. The organic phase, a solution of tributyl phosphate and sodium bis(trifluoromethylsulfonyl)imide (NaNTf2) was filled into porous membranes as the solid phase using an impregnation method to construct a supported ionic liquid membranes (SILMs) contactor for lithium extraction from simulated salt-lake brine. The feed and stripping phases of the contactor were a mixed Mg/Li solution and 0.5 mol/L HCl, respectively. The contactor operated continuously for 120 h. The results showed an HF membrane with an average pore size of 20.1 nm, porosity of 73.6 % and a breaking strength of 5.64 MPa. When the Mg/Li mass ratio in the feed was approximately 3.5, the mass transfer rate of Li+ and the separation factor (SFLi−Mg) obtained from the contactor with a packing density of 1.5 % were 0.468 μm/s and 15.86, respectively. After further increasing the mass ratio of the Mg/Li solution to 35 in the feed and the membrane packing density to 15 %, the mass transfer rate of Li+ and the SFLi−Mg increased to 0.623 μm/s and 30.8, respectively. This implies that the SILMs contactor with a high packing density of HF membrane showed good operating stability and enhanced ion extraction efficiency. The high performance was ascribed to the crown ether groups in 14C4PI achieving specific recognition of Li+ through the size-sieving effect. Specifically, the inter-molecular interaction between crown ether and ionic liquids (ILs) improved the stability of the filled ILs. Meanwhile, ILs provided ionic transfer channels and promoted the dehydration process of Li+, leading to a high SFLi−Mg. In addition, NaNTf2 adopted to replace traditional ILs prevented cation loss and provided an efficient and continuous method for extracting lithium from salt-lake. The above advantages are expected to achieve large-scale extraction of lithium ions.
{"title":"A hollow fiber supported ionic liquid membrane contactor for continuous extraction of lithium from high magnesium/lithium ratio brine","authors":"Bo Dong ,&nbsp;Junyuan Hua ,&nbsp;Jintao He ,&nbsp;Jiahui Du ,&nbsp;Jian Xiao ,&nbsp;Jianxin Li","doi":"10.1016/j.watres.2025.123451","DOIUrl":"10.1016/j.watres.2025.123451","url":null,"abstract":"<div><div>High-efficiency lithium (Li<sup>+</sup>) extraction from a salt-lake brine with a low Li concentration and a high Mg/Li mass ratio poses a great challenge owing to the great physical and chemical similarities between Mg<sup>2+</sup> and Li<sup>+</sup>. In this study, a hollow fiber (HF) membrane with an inside diameter of 0.872 mm and an outside diameter of 1.228 mm was fabricated using nonsolvent induce phase separation method with 14-crown-4 ether functionalized polyimide (14C4PI) as a polymer matrix. The organic phase, a solution of tributyl phosphate and sodium bis(trifluoromethylsulfonyl)imide (NaNTf<sub>2</sub>) was filled into porous membranes as the solid phase using an impregnation method to construct a supported ionic liquid membranes (SILMs) contactor for lithium extraction from simulated salt-lake brine. The feed and stripping phases of the contactor were a mixed Mg/Li solution and 0.5 mol/L HCl, respectively. The contactor operated continuously for 120 h. The results showed an HF membrane with an average pore size of 20.1 nm, porosity of 73.6 % and a breaking strength of 5.64 MPa. When the Mg/Li mass ratio in the feed was approximately 3.5, the mass transfer rate of Li<sup>+</sup> and the separation factor (SF<sub>Li−Mg</sub>) obtained from the contactor with a packing density of 1.5 % were 0.468 μm/s and 15.86, respectively. After further increasing the mass ratio of the Mg/Li solution to 35 in the feed and the membrane packing density to 15 %, the mass transfer rate of Li<sup>+</sup> and the SF<sub>Li−Mg</sub> increased to 0.623 μm/s and 30.8, respectively. This implies that the SILMs contactor with a high packing density of HF membrane showed good operating stability and enhanced ion extraction efficiency. The high performance was ascribed to the crown ether groups in 14C4PI achieving specific recognition of Li<sup>+</sup> through the size-sieving effect. Specifically, the inter-molecular interaction between crown ether and ionic liquids (ILs) improved the stability of the filled ILs. Meanwhile, ILs provided ionic transfer channels and promoted the dehydration process of Li<sup>+</sup>, leading to a high SF<sub>Li−Mg</sub>. In addition, NaNTf<sub>2</sub> adopted to replace traditional ILs prevented cation loss and provided an efficient and continuous method for extracting lithium from salt-lake. The above advantages are expected to achieve large-scale extraction of lithium ions.</div></div>","PeriodicalId":443,"journal":{"name":"Water Research","volume":"279 ","pages":"Article 123451"},"PeriodicalIF":11.4,"publicationDate":"2025-03-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143570093","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
A novel framework for tracking hydrological processes and identifying key factors in mountain-lowland mixed catchments: Implications of forty years of modeling for water management
IF 11.4 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2025-03-07 DOI: 10.1016/j.watres.2025.123424
Renhua Yan , Lingling Li , Junfeng Gao
Quantitative analysis of runoff, total suspended solids, and total nitrogen dynamics, along with the identification of key factors within catchments, is essential for accurately addressing issues related to turbid and polluted water. Nevertheless, their implementation encounters significant challenges when applied to a mixed catchment containing mountain areas and lowland polder regions, due to the highly heterogeneous hydrological behaviors and consequently the lack of an appropriate approach. Faced with this problem, this study developed a framework by coupling the Soil and Water Assessment Tool (SWAT) and improved Polder Hydrology and Nitrogen modelling System (PHNS), and Random Forest analysis method to track the spatio-temporal changes in runoff, total suspended solids, and total nitrogen loading and identify their environmental determinants in a representative mountain-lowland mixed catchment, southeastern China. The coupled model performed very well for runoff (R2≥0.90) and water quality variables (total suspended solids: R2≥0.88; total nitrogen: R2≥0.73) in both the calibration and validation periods, and showed improvements compared with standalone SWAT model. Forty years’ modelling results indicated that the upstream subbasins 15 (32.86 tonnes/ha/yr), 14 (33.96 tonnes/ha/yr), and 11 (32.32 tonnes/ha/yr) were the critical source areas for total suspended solids and total nitrogen. However, the downstream polder subbasins functioned as a sink for runoff, total suspended solids, and total nitrogen, exporting lower loading intensities. Precipitation and the proportion of slope of 0 to 30° were identified as the critical factors influencing runoff, total suspended solids, and total nitrogen. The proportion of water area also significantly, negatively influenced runoff and total suspended solids. This study provided a feasible method to investigate runoff, total suspended solids, and total nitrogen processes and their environmental factors’ impact, and thus identifying the critical source areas and targeted measures to control the non-point source pollution of mountain-lowland mixed catchments.
{"title":"A novel framework for tracking hydrological processes and identifying key factors in mountain-lowland mixed catchments: Implications of forty years of modeling for water management","authors":"Renhua Yan ,&nbsp;Lingling Li ,&nbsp;Junfeng Gao","doi":"10.1016/j.watres.2025.123424","DOIUrl":"10.1016/j.watres.2025.123424","url":null,"abstract":"<div><div>Quantitative analysis of runoff, total suspended solids, and total nitrogen dynamics, along with the identification of key factors within catchments, is essential for accurately addressing issues related to turbid and polluted water. Nevertheless, their implementation encounters significant challenges when applied to a mixed catchment containing mountain areas and lowland polder regions, due to the highly heterogeneous hydrological behaviors and consequently the lack of an appropriate approach. Faced with this problem, this study developed a framework by coupling the Soil and Water Assessment Tool (SWAT) and improved Polder Hydrology and Nitrogen modelling System (PHNS), and Random Forest analysis method to track the spatio-temporal changes in runoff, total suspended solids, and total nitrogen loading and identify their environmental determinants in a representative mountain-lowland mixed catchment, southeastern China. The coupled model performed very well for runoff (R<sup>2</sup>≥0.90) and water quality variables (total suspended solids: R<sup>2</sup>≥0.88; total nitrogen: R<sup>2</sup>≥0.73) in both the calibration and validation periods, and showed improvements compared with standalone SWAT model. Forty years’ modelling results indicated that the upstream subbasins 15 (32.86 tonnes/ha/yr), 14 (33.96 tonnes/ha/yr), and 11 (32.32 tonnes/ha/yr) were the critical source areas for total suspended solids and total nitrogen. However, the downstream polder subbasins functioned as a sink for runoff, total suspended solids, and total nitrogen, exporting lower loading intensities. Precipitation and the proportion of slope of 0 to 30° were identified as the critical factors influencing runoff, total suspended solids, and total nitrogen. The proportion of water area also significantly, negatively influenced runoff and total suspended solids. This study provided a feasible method to investigate runoff, total suspended solids, and total nitrogen processes and their environmental factors’ impact, and thus identifying the critical source areas and targeted measures to control the non-point source pollution of mountain-lowland mixed catchments.</div></div>","PeriodicalId":443,"journal":{"name":"Water Research","volume":"279 ","pages":"Article 123424"},"PeriodicalIF":11.4,"publicationDate":"2025-03-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143570094","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Molecular-level insights into dissolved organic matter during Ulva prolifera degradation and its regulation on the environmental behaviour of the organic pollutant tributyl phosphate
IF 11.4 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2025-03-07 DOI: 10.1016/j.watres.2025.123436
Hanwen Hu , Chengmin Wang , Xuexi Tang , Ying Wang , Xiaoyang Jian , Suyang Liu , Xinxin Zhang
Macroalgal blooms have frequently occurred in coastal waters, and a large amount of algogenic dissolved organic matter (DOM) is input into seawater as macroalgae degraded. It undergoes continuous changes under microbial degradation; however, the impact of microbially-modified marine DOM on the environmental behaviour of organic pollutants remains underexplored. This study focused on Ulva prolifera, the dominant species in green tides, and investigated the molecular diversity of DOM from U. prolifera degradation over a 100-day period and the role of DOM at different time points in the adsorption of organophosphate flame retardants onto goethite. Our findings revealed that dissolved organic carbon (DOC) in seawater increased sharply during the first two weeks, followed by a rapid decline, and eventually reached a stable level within 100 days. Multi-spectrum analysis and Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS), along with the results of spectral analysis, indicated an increase in the humification and aromaticity of DOM, accompanied by the transformation of protein components, suggesting a decrease in DOM bioavailability. Microbial abundance aligned with DOC trends, and 16S rRNA results revealed significant shifts in the microbial community during DOM transformation. A strong correlation between fluorescent DOM groups and microbial diversity was observed, and co-occurrence network analysis further identified Alteromonas and Vibrio as major contributors to DOM chemical diversity. The introduction of U. prolifera DOM reduced available surface sites on goethite, inhibiting the adsorption rate of tributyl phosphate (TnBP) in batch sorption experiments. However, this competitive sorption effect was mitigated by co-sorption, as DOM could bind with TnBP, explaining the observed increase in adsorption capacity. Redundancy analysis and verification tests suggested protein-like DOM components play a crucial role in sorption, and microbial transformation of DOM-proteins could diminish this effect. These findings underscore the importance of macroalgal DOM in influencing the environmental behaviour of organic pollutants and could supply a supplement about the ecological effect about macroalgal blooms.
{"title":"Molecular-level insights into dissolved organic matter during Ulva prolifera degradation and its regulation on the environmental behaviour of the organic pollutant tributyl phosphate","authors":"Hanwen Hu ,&nbsp;Chengmin Wang ,&nbsp;Xuexi Tang ,&nbsp;Ying Wang ,&nbsp;Xiaoyang Jian ,&nbsp;Suyang Liu ,&nbsp;Xinxin Zhang","doi":"10.1016/j.watres.2025.123436","DOIUrl":"10.1016/j.watres.2025.123436","url":null,"abstract":"<div><div>Macroalgal blooms have frequently occurred in coastal waters, and a large amount of algogenic dissolved organic matter (DOM) is input into seawater as macroalgae degraded. It undergoes continuous changes under microbial degradation; however, the impact of microbially-modified marine DOM on the environmental behaviour of organic pollutants remains underexplored. This study focused on Ulva prolifera, the dominant species in green tides, and investigated the molecular diversity of DOM from U. prolifera degradation over a 100-day period and the role of DOM at different time points in the adsorption of organophosphate flame retardants onto goethite. Our findings revealed that dissolved organic carbon (DOC) in seawater increased sharply during the first two weeks, followed by a rapid decline, and eventually reached a stable level within 100 days. Multi-spectrum analysis and Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS), along with the results of spectral analysis, indicated an increase in the humification and aromaticity of DOM, accompanied by the transformation of protein components, suggesting a decrease in DOM bioavailability. Microbial abundance aligned with DOC trends, and 16S rRNA results revealed significant shifts in the microbial community during DOM transformation. A strong correlation between fluorescent DOM groups and microbial diversity was observed, and co-occurrence network analysis further identified Alteromonas and Vibrio as major contributors to DOM chemical diversity. The introduction of U<em>. prolifera</em> DOM reduced available surface sites on goethite, inhibiting the adsorption rate of tributyl phosphate (TnBP) in batch sorption experiments. However, this competitive sorption effect was mitigated by co-sorption, as DOM could bind with TnBP, explaining the observed increase in adsorption capacity. Redundancy analysis and verification tests suggested protein-like DOM components play a crucial role in sorption, and microbial transformation of DOM-proteins could diminish this effect. These findings underscore the importance of macroalgal DOM in influencing the environmental behaviour of organic pollutants and could supply a supplement about the ecological effect about macroalgal blooms.</div></div>","PeriodicalId":443,"journal":{"name":"Water Research","volume":"279 ","pages":"Article 123436"},"PeriodicalIF":11.4,"publicationDate":"2025-03-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143570092","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
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