Pub Date : 2025-03-12DOI: 10.1016/j.watres.2025.123493
Yanjie Wang, Yifan Liu, Changfu Hao, Yan Li, Yang Liu, Bisheng Lai, Haoran Zhu, Kaixiong Yang
Wastewater treatment plants (WWTPs) have been proposed as pivotal convergence points for microplastics (MPs) and hotspots of bacterial pathogens. In this study, the characteristics of MPs and bacteria in the sewage/sludge were investigated and their relationship was formulated. Meanwhile, this study innovatively focuses on the impact of MPs on microbial aerosolization process in WWTP. MPs and pathogenic bacteria were identified in sewage/sludge samples from all treatment steps, in which the levels and compositions of them vary. However, Bacillus, Planifilum, Achromobacter, and Geobacillus were the dominant genera in bioaerosol samples. The dominant shape of MPs was fibers and fragments. The main size range of MPs were 0.5 - 1 mm, with the primary type of polyethylene and polypropylene. White was the most prevalent color. Furthermore, a significant correlation between MPs and bacterial community structure in sewage/sludge was observed. The abundance and some characteristics of MPs showed positive correlations with the relative abundances of some potential pathogens, including Bacillus, Pseudomonas, Staphylococcus, Acinetobacter and Achromobacter. Aeration experiments demonstrated that the presence of MPs exerted an influence on the microbial aerosolization process. Collectively, this study provides a better understanding of the relationship between MPs and bacterial structures in a WWTP and offers new insights to the role of MPs on the microbial aerosolization process. The findings will provide a basis for the control and reduction of MPs and bacterial pathogens in WWTPs.
{"title":"Microplastics in wastewater treatment plant: characterization of changes, influencing factors, and their impact on the spatial distribution of pathogenic bacteria","authors":"Yanjie Wang, Yifan Liu, Changfu Hao, Yan Li, Yang Liu, Bisheng Lai, Haoran Zhu, Kaixiong Yang","doi":"10.1016/j.watres.2025.123493","DOIUrl":"https://doi.org/10.1016/j.watres.2025.123493","url":null,"abstract":"Wastewater treatment plants (WWTPs) have been proposed as pivotal convergence points for microplastics (MPs) and hotspots of bacterial pathogens. In this study, the characteristics of MPs and bacteria in the sewage/sludge were investigated and their relationship was formulated. Meanwhile, this study innovatively focuses on the impact of MPs on microbial aerosolization process in WWTP. MPs and pathogenic bacteria were identified in sewage/sludge samples from all treatment steps, in which the levels and compositions of them vary. However, <em>Bacillus, Planifilum, Achromobacter</em>, and <em>Geobacillus</em> were the dominant genera in bioaerosol samples. The dominant shape of MPs was fibers and fragments. The main size range of MPs were 0.5 - 1 mm, with the primary type of polyethylene and polypropylene. White was the most prevalent color. Furthermore, a significant correlation between MPs and bacterial community structure in sewage/sludge was observed. The abundance and some characteristics of MPs showed positive correlations with the relative abundances of some potential pathogens, including <em>Bacillus, Pseudomonas, Staphylococcus, Acinetobacter</em> and <em>Achromobacter</em>. Aeration experiments demonstrated that the presence of MPs exerted an influence on the microbial aerosolization process. Collectively, this study provides a better understanding of the relationship between MPs and bacterial structures in a WWTP and offers new insights to the role of MPs on the microbial aerosolization process. The findings will provide a basis for the control and reduction of MPs and bacterial pathogens in WWTPs.","PeriodicalId":443,"journal":{"name":"Water Research","volume":"16 1","pages":""},"PeriodicalIF":12.8,"publicationDate":"2025-03-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143608143","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}
Pub Date : 2025-03-12DOI: 10.1016/j.watres.2025.123487
Magdalena M. Mrokowska, Karolina Dzień, Anna Krztoń-Maziopa
The settling behaviour of microplastics (MPs) governs their residence time and bioavailability in the water column. Despite significant research efforts on the hydrodynamics of MPs in various aquatic environments, little attention has been given to MPs sinking in seawater enriched with mucus formed by exopolymers (EPSs) excessively secreted by microorganisms during algal blooms. These blooms often develop in density-stratified seawater and can rheologically modify the system by introducing a non-Newtonian EPS-rich layer to the Newtonian seawater column with a typical content of EPSs. In this study, we investigated the previously unaddressed role of rheological stratification that forms at the periphery of the algal bloom region in MPs sinking process. Our laboratory experiments revealed that variations in viscosity and viscoelasticity between Newtonian and non-Newtonian layers significantly impact MPs sinking velocity and orientation, often outweighing the effects of density stratification. Results demonstrated that the sinking velocity of MPs decreased in the non-Newtonian layer leading to residence times up to five times longer than in the Newtonian layer, showing a clear dependence on the viscosity difference between the two layers. Meanwhile, we identified the orientation instabilities of MPs enhanced with increasing EPS content. This study revealed previously unaddressed hydrodynamic effects in rheologically stratified seawater that may intensify MPs accumulation and their interactions with the ecosystem. This could help explain MPs fate in algal bloom-afflicted regions.
{"title":"Effects of rheologically stratified seawater during algal bloom on sinking dynamics of microplastics","authors":"Magdalena M. Mrokowska, Karolina Dzień, Anna Krztoń-Maziopa","doi":"10.1016/j.watres.2025.123487","DOIUrl":"https://doi.org/10.1016/j.watres.2025.123487","url":null,"abstract":"The settling behaviour of microplastics (MPs) governs their residence time and bioavailability in the water column. Despite significant research efforts on the hydrodynamics of MPs in various aquatic environments, little attention has been given to MPs sinking in seawater enriched with mucus formed by exopolymers (EPSs) excessively secreted by microorganisms during algal blooms. These blooms often develop in density-stratified seawater and can rheologically modify the system by introducing a non-Newtonian EPS-rich layer to the Newtonian seawater column with a typical content of EPSs. In this study, we investigated the previously unaddressed role of rheological stratification that forms at the periphery of the algal bloom region in MPs sinking process. Our laboratory experiments revealed that variations in viscosity and viscoelasticity between Newtonian and non-Newtonian layers significantly impact MPs sinking velocity and orientation, often outweighing the effects of density stratification. Results demonstrated that the sinking velocity of MPs decreased in the non-Newtonian layer leading to residence times up to five times longer than in the Newtonian layer, showing a clear dependence on the viscosity difference between the two layers. Meanwhile, we identified the orientation instabilities of MPs enhanced with increasing EPS content. This study revealed previously unaddressed hydrodynamic effects in rheologically stratified seawater that may intensify MPs accumulation and their interactions with the ecosystem. This could help explain MPs fate in algal bloom-afflicted regions.","PeriodicalId":443,"journal":{"name":"Water Research","volume":"86 1 1","pages":""},"PeriodicalIF":12.8,"publicationDate":"2025-03-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143599413","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}
Wastewater-based epidemiological (WBE) surveillance has emerged as a crucial tool for monitoring infectious diseases within communities. However, its broader application is frequently constrained by the high costs, labor-intensive processes, and extended timeframes required for sample collection, transportation, and processing. Aptamer-based biosensors offer a promising alternative, leveraging the specific binding properties of aptamers to biomolecules for the on-site and rapid quantification of disease biomarkers in wastewater. This review systematically evaluates recent advancements in the application of aptamer-based biosensors for the detection of key pathogens, including SARS-CoV-2, influenza viruses, and norovirus, within wastewater matrices. The discussion encompasses the technical stability and reliability of signal transmission associated with these biosensors, as well as the current challenges faced in real-world implementation. Noteworthy progress has been made in the development of these biosensors for WBE, achieving detection limits as low as femtomolar (fM) levels in buffer and linear dynamic ranges extending up to five orders of magnitude for viruses such as influenza and SARS-CoV-2. Despite this progress, considerable hurdles remain to be addressed before these technologies can be effectively deployed in practical settings, especially within complex wastewater environments. Key factors affecting detection performance include matrix interference, environmental variability, and the diminished stability of both viral targets and aptamer-target interactions in wastewater. This review not only highlights these challenges but also outlines potential avenues for future research aimed at enhancing the functionality and applicability of aptamer-based biosensors in WBE, ultimately contributing to more effective public health surveillance and disease monitoring strategies.
{"title":"Aptamer-based biosensors for wastewater surveillance of influenza virus, SARS-CoV-2, and norovirus: A comprehensive review","authors":"Yilei Wang, Mohan Amarasiri, Wakana Oishi, Masayasu Kuwahara, Yuka Kataoka, Hiroki Kurita, Fumio Narita, Rong Chen, Qian Li, Daisuke Sano","doi":"10.1016/j.watres.2025.123484","DOIUrl":"https://doi.org/10.1016/j.watres.2025.123484","url":null,"abstract":"Wastewater-based epidemiological (WBE) surveillance has emerged as a crucial tool for monitoring infectious diseases within communities. However, its broader application is frequently constrained by the high costs, labor-intensive processes, and extended timeframes required for sample collection, transportation, and processing. Aptamer-based biosensors offer a promising alternative, leveraging the specific binding properties of aptamers to biomolecules for the on-site and rapid quantification of disease biomarkers in wastewater. This review systematically evaluates recent advancements in the application of aptamer-based biosensors for the detection of key pathogens, including SARS-CoV-2, influenza viruses, and norovirus, within wastewater matrices. The discussion encompasses the technical stability and reliability of signal transmission associated with these biosensors, as well as the current challenges faced in real-world implementation. Noteworthy progress has been made in the development of these biosensors for WBE, achieving detection limits as low as femtomolar (fM) levels in buffer and linear dynamic ranges extending up to five orders of magnitude for viruses such as influenza and SARS-CoV-2. Despite this progress, considerable hurdles remain to be addressed before these technologies can be effectively deployed in practical settings, especially within complex wastewater environments. Key factors affecting detection performance include matrix interference, environmental variability, and the diminished stability of both viral targets and aptamer-target interactions in wastewater. This review not only highlights these challenges but also outlines potential avenues for future research aimed at enhancing the functionality and applicability of aptamer-based biosensors in WBE, ultimately contributing to more effective public health surveillance and disease monitoring strategies.","PeriodicalId":443,"journal":{"name":"Water Research","volume":"14 1","pages":""},"PeriodicalIF":12.8,"publicationDate":"2025-03-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143608142","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}
Benzothiazole was taken as a simple emerging aromatic heterocyclic contaminant as model compounds for analyzing multi-element isotope (ME-CSIA) fractionation (2H, 13C, 15N and 33/34S) for the first time, in order to obtain information on the reaction mechanism upon sulfate and hydroxyl radical reactions and photolysis. The sulfur isotope effects 33/34S to allow to explore reactions mechanisms with respect to mass dependent and independent kinetic isotope effect. For compound specific isotope analysis for 2H, 13C, and 15N using GC-pyrolysis and combustion IRMS techniques were applied and for 33/34S isotope analysis a novel approach using GC- multi collector ICPMS were developed. The multi-element fractionation factors of the radical reactions were obtained to characterize the first irreversible degradation step in order explore their potential to analyze radical oxidation processes in technical and natural systems. The hydroxyl radical reactions yield small carbon (εC = −0.67 ± 0.06‰), large hydrogen (εH = −8.8 ± 0.9‰), and negligible nitrogen and sulfur isotope fractionations as cleavage of the C−H bond the benzene ring is the first irreversible step. The heat-activated persulphate oxidation at pH = 2, dominated by SO4•− radicals were associated with significant for C (εC = −1.56 ± 0.09‰), N (εN = 1.08 ± 0.05‰), and S (ε33S = −0.6 ± 0.04‰, ε34S = −1.1 ± 0.09‰), and negligible for H isotope fraction, indicating cleavage of the C−S bond.
{"title":"Multi-element Compound-Specific Stable Isotope Analysis (2H, 13C, 15N, 33/34S) to characterize the mechanism of sulfate and hydroxyl radical reaction and photolysis of benzothiazole","authors":"Haiyan Yu, Limin Ma, Steffen Kümmel, Xiao Liu, Thomas Schaefer, Hartmut Herrmann, Hans-Hermann Richnow","doi":"10.1016/j.watres.2025.123479","DOIUrl":"https://doi.org/10.1016/j.watres.2025.123479","url":null,"abstract":"Benzothiazole was taken as a simple emerging aromatic heterocyclic contaminant as model compounds for analyzing multi-element isotope (ME-CSIA) fractionation (<sup>2</sup>H, <sup>13</sup>C, <sup>15</sup>N and <sup>33/34</sup>S) for the first time, in order to obtain information on the reaction mechanism upon sulfate and hydroxyl radical reactions and photolysis. The sulfur isotope effects <sup>33</sup>/<sup>34</sup>S to allow to explore reactions mechanisms with respect to mass dependent and independent kinetic isotope effect. For compound specific isotope analysis for <sup>2</sup>H, <sup>13</sup>C, and <sup>15</sup>N using GC-pyrolysis and combustion IRMS techniques were applied and for <sup>33/34</sup>S isotope analysis a novel approach using GC- multi collector ICPMS were developed. The multi-element fractionation factors of the radical reactions were obtained to characterize the first irreversible degradation step in order explore their potential to analyze radical oxidation processes in technical and natural systems. The hydroxyl radical reactions yield small carbon (<em>ε</em><sub>C</sub> = −0.67 ± 0.06‰), large hydrogen (<em>ε</em><sub>H</sub> = −8.8 ± 0.9‰), and negligible nitrogen and sulfur isotope fractionations as cleavage of the C−H bond the benzene ring is the first irreversible step. The heat-activated persulphate oxidation at pH = 2, dominated by SO<sub>4</sub> <sup>•−</sup> radicals were associated with significant for C (<em>ε</em><sub>C</sub> = −1.56 ± 0.09‰), N (<em>ε</em><sub>N</sub> = 1.08 ± 0.05‰), and S (<em>ε</em><sup>33</sup>S = −0.6 ± 0.04‰, <em>ε</em><sup>34</sup>S = −1.1 ± 0.09‰), and negligible for H isotope fraction, indicating cleavage of the C−S bond.","PeriodicalId":443,"journal":{"name":"Water Research","volume":"68 1","pages":""},"PeriodicalIF":12.8,"publicationDate":"2025-03-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143589957","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}
Pub Date : 2025-03-11DOI: 10.1016/j.watres.2025.123464
L. Engelbart, S. Bieger, K. Thompson, L. Fischer, T. Bader, M. Kramer, S. Haderlein, A. Röhnelt, P. Martin, D. Buchner, R. Bloch, H. Rügner, C. Huhn
The herbicide glyphosate and aminomethyl phosphonic acid (AMPA), a transformation product of glyphosate and other aminopholyphosphonates are widespread pollutants in European rivers. We recently showed that besides rain-driven input after agricultural or urban herbicide application, municipal wastewater significantly contributes to glyphosate contamination in European rivers. The rather constant mass fluxes over the year, made an explanation by herbicide applications difficult. In our search for a new source of glyphosate and AMPA, we here provide experimental evidence that a certain aminopolyphosphonate, used as antiscalant and bleach stabilizer in household detergents and numerous industrial processes, is a precursor of both glyphosate and AMPA. During incubation experiments with diethylenetriamine penta(methylene phosphonic acid) (DTPMP) in fresh activated sludge, we observed the formation of glyphosate with yields ranging from 0.017 to 0.040 mol% and formation of AMPA in the range of 0.402 to 1.72 mol% after 72 h. Both compounds are formed from DTPMP and possible intermediates, but they are also further transformed themselves in consecutive reactions. Glyphosate formation from DTPMP was further proven by incubating 13C-labeled DTPMP, which transformed into 13C-glyphosate and 13C-AMPA. The addition of DTPMP to azide-treated activated sludge yielded similar or even higher glyphosate and AMPA concentrations indicating that abiotic processes dominate the transformation process. In order to judge the relevance of this in-situ formation of glyphosate and AMPA from the laundry additive DTPMP, we estimated the average concentrations in wastewater.
{"title":"In-situ formation of glyphosate and AMPA in activated sludge from phosphonates used as antiscalants and bleach stabilizers in households and industry","authors":"L. Engelbart, S. Bieger, K. Thompson, L. Fischer, T. Bader, M. Kramer, S. Haderlein, A. Röhnelt, P. Martin, D. Buchner, R. Bloch, H. Rügner, C. Huhn","doi":"10.1016/j.watres.2025.123464","DOIUrl":"https://doi.org/10.1016/j.watres.2025.123464","url":null,"abstract":"The herbicide glyphosate and aminomethyl phosphonic acid (AMPA), a transformation product of glyphosate and other aminopholyphosphonates are widespread pollutants in European rivers. We recently showed that besides rain-driven input after agricultural or urban herbicide application, municipal wastewater significantly contributes to glyphosate contamination in European rivers. The rather constant mass fluxes over the year, made an explanation by herbicide applications difficult. In our search for a new source of glyphosate and AMPA, we here provide experimental evidence that a certain aminopolyphosphonate, used as antiscalant and bleach stabilizer in household detergents and numerous industrial processes, is a precursor of both glyphosate and AMPA. During incubation experiments with diethylenetriamine penta(methylene phosphonic acid) (DTPMP) in fresh activated sludge, we observed the formation of glyphosate with yields ranging from 0.017 to 0.040 mol% and formation of AMPA in the range of 0.402 to 1.72 mol% after 72 h. Both compounds are formed from DTPMP and possible intermediates, but they are also further transformed themselves in consecutive reactions. Glyphosate formation from DTPMP was further proven by incubating <sup>13</sup>C-labeled DTPMP, which transformed into <sup>13</sup>C-glyphosate and <sup>13</sup>C-AMPA. The addition of DTPMP to azide-treated activated sludge yielded similar or even higher glyphosate and AMPA concentrations indicating that abiotic processes dominate the transformation process. In order to judge the relevance of this in-situ formation of glyphosate and AMPA from the laundry additive DTPMP, we estimated the average concentrations in wastewater.","PeriodicalId":443,"journal":{"name":"Water Research","volume":"5 1","pages":""},"PeriodicalIF":12.8,"publicationDate":"2025-03-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143599133","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}
Pub Date : 2025-03-11DOI: 10.1016/j.watres.2025.123435
Qiuyun Lu , Deepak Panchal , Lingling Yang , Ziya Saedi , Mohamed Gamal El-Din , Xuehua Zhang
Elimination of stubborn organic micropollutants from water is crucial for bioaccumulation prevention and ecosystem protection. Cold plasma activation technology is a clean, sustainable, and highly effective approach to the degradation of micropollutants and pathogens in contaminated water. In this study, we focus on understanding the processes of simultaneous degradation of multiple micropollutants (8 types at maximum) in flowing water by the recently developed microbubble-enhanced cold plasma activation (MB-CPA) technology. The degradation of micropollutants with the treatment time was analyzed by using ultrahigh performance liquid chromatography coupled to a triple quadrupole mass spectrometer (UHPLC-QQQ-MS). We found that the degradation efficiencies of all compounds increase rapidly under strong activation conditions that can lead to above 98% removal of a model compound. After long treatment duration or at a fast flow rate, the removal efficiency was sufficiently high for all compounds that were either easy or hard to degrade. The large variation in degradation efficiencies was present under mild activation conditions. The electron spinning resonance measurements reveal a greater abundance of hydroxyl radicals in treated synthetic river water than pure water, highlighting the effects of water matrix on the degradation efficiency. The understanding from this work may help to design the activation process and minimize the energy consumption for the simultaneous elimination of pollutants in diverse and complex water bodies by cold plasma technology.
{"title":"Simultaneous degradation of multiple micropollutants in flowing water by mild and strong microbubble-enhanced cold plasma activation","authors":"Qiuyun Lu , Deepak Panchal , Lingling Yang , Ziya Saedi , Mohamed Gamal El-Din , Xuehua Zhang","doi":"10.1016/j.watres.2025.123435","DOIUrl":"10.1016/j.watres.2025.123435","url":null,"abstract":"<div><div>Elimination of stubborn organic micropollutants from water is crucial for bioaccumulation prevention and ecosystem protection. Cold plasma activation technology is a clean, sustainable, and highly effective approach to the degradation of micropollutants and pathogens in contaminated water. In this study, we focus on understanding the processes of simultaneous degradation of multiple micropollutants (8 types at maximum) in flowing water by the recently developed microbubble-enhanced cold plasma activation (MB-CPA) technology. The degradation of micropollutants with the treatment time was analyzed by using ultrahigh performance liquid chromatography coupled to a triple quadrupole mass spectrometer (UHPLC-QQQ-MS). We found that the degradation efficiencies of all compounds increase rapidly under strong activation conditions that can lead to above 98% removal of a model compound. After long treatment duration or at a fast flow rate, the removal efficiency was sufficiently high for all compounds that were either easy or hard to degrade. The large variation in degradation efficiencies was present under mild activation conditions. The electron spinning resonance measurements reveal a greater abundance of hydroxyl radicals in treated synthetic river water than pure water, highlighting the effects of water matrix on the degradation efficiency. The understanding from this work may help to design the activation process and minimize the energy consumption for the simultaneous elimination of pollutants in diverse and complex water bodies by cold plasma technology.</div></div>","PeriodicalId":443,"journal":{"name":"Water Research","volume":"280 ","pages":"Article 123435"},"PeriodicalIF":11.4,"publicationDate":"2025-03-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143599130","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}
Pub Date : 2025-03-11DOI: 10.1016/j.watres.2025.123483
Bo Deng , Zihe Ren , Qiang Li , Zhijian Zhang , Chao Xu , Panpan Wang , Heping Zhao , Qiaoxia Yuan
Intestinal microbiota and metal regulatory proteins (MRPs) underlie the transformation of heavy metals (HMs) by the black soldier fly larvae (BSFL), but the mechanisms involved are still not fully defined. Here, using 16S rRNA and metagenomics-assisted tracing, we found that zinc (Zn) and chromium (Cr) stress led to enrichment of Proteobacteria in the BSFL intestine. Support of Proteobacteria also led to increased levels of the Zn transporter proteins ZnuC/B/A and the Zn efflux proteins zntR/A. Meanwhile, the genes MltE, CitT, and SLT, which mediate the citric acid cycle, were also significantly up-regulated and involved in the cellular uptake of Cr. Although Zn and Cr stress affected the expression of antibiotic resistance genes and pathogenic genes, the BSFL intestine tended to form stable microbial communities (MCs) to transform HMs through a mechanism driven by ZupT and chrA. In addition, the expression of SCARB1 and LdcA was significantly down-regulated by acute HMs stimulation, but BSFL were still able to complete the life cycle. Therefore, we determined the protective role of MCs and MRPs on BSFL during the transformation of HMs.
{"title":"Black soldier fly larvae mediate Zinc and Chromium transformation through the ZnuCBA and citric acid cycle system","authors":"Bo Deng , Zihe Ren , Qiang Li , Zhijian Zhang , Chao Xu , Panpan Wang , Heping Zhao , Qiaoxia Yuan","doi":"10.1016/j.watres.2025.123483","DOIUrl":"10.1016/j.watres.2025.123483","url":null,"abstract":"<div><div>Intestinal microbiota and metal regulatory proteins (MRPs) underlie the transformation of heavy metals (HMs) by the black soldier fly larvae (BSFL), but the mechanisms involved are still not fully defined. Here, using 16S rRNA and metagenomics-assisted tracing, we found that zinc (Zn) and chromium (Cr) stress led to enrichment of Proteobacteria in the BSFL intestine. Support of Proteobacteria also led to increased levels of the Zn transporter proteins ZnuC/B/A and the Zn efflux proteins zntR/A. Meanwhile, the genes MltE, CitT, and SLT, which mediate the citric acid cycle, were also significantly up-regulated and involved in the cellular uptake of Cr. Although Zn and Cr stress affected the expression of antibiotic resistance genes and pathogenic genes, the BSFL intestine tended to form stable microbial communities (MCs) to transform HMs through a mechanism driven by ZupT and chrA. In addition, the expression of SCARB1 and LdcA was significantly down-regulated by acute HMs stimulation, but BSFL were still able to complete the life cycle. Therefore, we determined the protective role of MCs and MRPs on BSFL during the transformation of HMs.</div></div>","PeriodicalId":443,"journal":{"name":"Water Research","volume":"280 ","pages":"Article 123483"},"PeriodicalIF":11.4,"publicationDate":"2025-03-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143599132","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}
The removal of complexed Ni from wastewater typically requires advanced oxidation processes for decomplexation, followed by chemical precipitation or adsorption steps. Simplifying this process while meeting stringent discharge standards remains challenging. Here, we developed a one-step O3/H2O2/Fe0 system for the rapid and complete removal of Ni(II)-EDTA. In this system, Ni(II)-EDTA undergoes decomplexation and the resulting Ni2+ can be subsequently removed. Through this two-stage process, the concentration of total Ni can be decreased to below 0.1 mg/L at pH0 4.0-8.0. The O3/H2O2/Fe0 system generated multiple reactive oxidizing species, i.e., HO•, O2•−, 1O2, and Fe(IV). The probe method suggested Fe0 enhanced the production of 1O2 and Fe(IV), indicating their significant roles in this system. In the decomplexation stage, combined experimental evidence, including chemiluminescence, revealed the formation of Ni(IV) species. It progressively degraded into smaller chelated Ni(IV) intermediates and ultimately converted to Ni2+ and Ni(II/III) hydroxides. In the second stage, the Ni(II/III) hydroxides formed in the first stage catalyzed the oxidative removal of the Ni2+, resulting in final products composed of Ni(II/III) hydroxides. The H2O2 could favor the generation of Ni(II/III) hydroxides in the first stage, enhancing the subsequential removal of the Ni2+. These results can lead to a promising strategy for the removal and recovery of complex Ni from industrial wastewater.
{"title":"One-step rapid and complete removal of Ni(II)-EDTA by O3/H2O2/Fe0 process: The role of high-valent Ni species","authors":"Peixuan Yu, Huixin Shao, Yiran Feng, Yabo Liu, Peng Fan, Hejie Qin, Xiaohong Guan","doi":"10.1016/j.watres.2025.123459","DOIUrl":"https://doi.org/10.1016/j.watres.2025.123459","url":null,"abstract":"The removal of complexed Ni from wastewater typically requires advanced oxidation processes for decomplexation, followed by chemical precipitation or adsorption steps. Simplifying this process while meeting stringent discharge standards remains challenging. Here, we developed a one-step O<sub>3</sub>/H<sub>2</sub>O<sub>2</sub>/Fe<sup>0</sup> system for the rapid and complete removal of Ni(II)-EDTA. In this system, Ni(II)-EDTA undergoes decomplexation and the resulting Ni<sup>2+</sup> can be subsequently removed. Through this two-stage process, the concentration of total Ni can be decreased to below 0.1 mg/L at pH<sub>0</sub> 4.0-8.0. The O<sub>3</sub>/H<sub>2</sub>O<sub>2</sub>/Fe<sup>0</sup> system generated multiple reactive oxidizing species, i.e., HO<sup>•</sup>, O<sub>2</sub><sup>•−</sup>, <sup>1</sup>O<sub>2</sub>, and Fe(IV). The probe method suggested Fe<sup>0</sup> enhanced the production of <sup>1</sup>O<sub>2</sub> and Fe(IV), indicating their significant roles in this system. In the decomplexation stage, combined experimental evidence, including chemiluminescence, revealed the formation of Ni(IV) species. It progressively degraded into smaller chelated Ni(IV) intermediates and ultimately converted to Ni<sup>2+</sup> and Ni(II/III) hydroxides. In the second stage, the Ni(II/III) hydroxides formed in the first stage catalyzed the oxidative removal of the Ni<sup>2+</sup>, resulting in final products composed of Ni(II/III) hydroxides. The H<sub>2</sub>O<sub>2</sub> could favor the generation of Ni(II/III) hydroxides in the first stage, enhancing the subsequential removal of the Ni<sup>2+</sup>. These results can lead to a promising strategy for the removal and recovery of complex Ni from industrial wastewater.","PeriodicalId":443,"journal":{"name":"Water Research","volume":"14 1","pages":""},"PeriodicalIF":12.8,"publicationDate":"2025-03-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143599131","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}
Pub Date : 2025-03-10DOI: 10.1016/j.watres.2025.123476
Aonan Yang , Haiyan Pei , Ming Zhang , Yan Jin , Hangzhou Xu
Toxic blooms of benthic cyanobacteria greatly threaten freshwater ecological health and drinking water safety. Meanwhile, microplastic pollution is becoming increasingly severe and microplastics accumulate in large quantities at the bottom of lakes and rivers, widely coexisting with algae. However, impacts of microplastics on benthic cyanobacteria are still unknown. This study investigated effects of microplastic polyethylene terephthalate (PET) — which is commonly found at the bottom of lakes and rivers — and its leachate at environmentally relevant concentration (0.3 mg/L) and high exposure concentration (3.0 mg/L) on typical benthic cyanobacteria (Oscillatoria sp. and Pseudanabaena sp.), and clarified the related molecular mechanisms through transcriptomic analysis. Results show that PET or PET leachate (PET-L) can promote benthic cyanobacterial growth and promotive effect of PET-L is more obvious than that of PET system. Promotion effect of PET or PET-L is more significant at environmentally relevant concentration (39–63 % increase compared with the control) compared with high exposure concentration (21–58 % increase compared with the control). In the presence of PET or PET-L, due to an increase in the number of cyanobacterial cells, concentrations of harmful metabolites (cylindrospermopsin, geosmin, and 2-methylisoborneol) in water also increased. Although PET particles may not be conducive to benthic cyanobacterial growth due to shading effect and mechanical damage, photosynthetic efficiency of algae was improved and dysregulated genes related to photosynthesis and extracellular transport of glycolipid were upregulated according to transcriptome analysis. Moreover, PET decomposition components, such as terephthalic acid and ethylene glycol, may be able to serve as carbon sources for cyanobacterial growth. Upregulation of genes associated with glycolysis, oxidative phosphorylation, and translation revealed that PET can promote the growth of benthic cyanobacteria. This study has important value in evaluating the impact of benthic cyanobacteria on aquatic ecological health and drinking water safety with the coexistence of microplastics.
{"title":"Molecular mechanisms by which polyethylene terephthalate (PET) microplastic and PET leachate promote the growth of benthic cyanobacteria","authors":"Aonan Yang , Haiyan Pei , Ming Zhang , Yan Jin , Hangzhou Xu","doi":"10.1016/j.watres.2025.123476","DOIUrl":"10.1016/j.watres.2025.123476","url":null,"abstract":"<div><div>Toxic blooms of benthic cyanobacteria greatly threaten freshwater ecological health and drinking water safety. Meanwhile, microplastic pollution is becoming increasingly severe and microplastics accumulate in large quantities at the bottom of lakes and rivers, widely coexisting with algae. However, impacts of microplastics on benthic cyanobacteria are still unknown. This study investigated effects of microplastic polyethylene terephthalate (PET) — which is commonly found at the bottom of lakes and rivers — and its leachate at environmentally relevant concentration (0.3 mg/L) and high exposure concentration (3.0 mg/L) on typical benthic cyanobacteria (<em>Oscillatoria</em> sp. and <em>Pseudanabaena</em> sp.), and clarified the related molecular mechanisms through transcriptomic analysis. Results show that PET or PET leachate (PET-L) can promote benthic cyanobacterial growth and promotive effect of PET-L is more obvious than that of PET system. Promotion effect of PET or PET-L is more significant at environmentally relevant concentration (39–63 % increase compared with the control) compared with high exposure concentration (21–58 % increase compared with the control). In the presence of PET or PET-L, due to an increase in the number of cyanobacterial cells, concentrations of harmful metabolites (cylindrospermopsin, geosmin, and 2-methylisoborneol) in water also increased. Although PET particles may not be conducive to benthic cyanobacterial growth due to shading effect and mechanical damage, photosynthetic efficiency of algae was improved and dysregulated genes related to photosynthesis and extracellular transport of glycolipid were upregulated according to transcriptome analysis. Moreover, PET decomposition components, such as terephthalic acid and ethylene glycol, may be able to serve as carbon sources for cyanobacterial growth. Upregulation of genes associated with glycolysis, oxidative phosphorylation, and translation revealed that PET can promote the growth of benthic cyanobacteria. This study has important value in evaluating the impact of benthic cyanobacteria on aquatic ecological health and drinking water safety with the coexistence of microplastics.</div></div>","PeriodicalId":443,"journal":{"name":"Water Research","volume":"280 ","pages":"Article 123476"},"PeriodicalIF":11.4,"publicationDate":"2025-03-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143589956","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}
Hexavalent chromium (Cr(VI)) is one of the most rigorously regulated contaminants frequently detected in surface and groundwater. Magnetic iron sulfides are naturally abundant, environmentally friendly materials ideal for the removal of Cr(VI) from contaminated water, but the high-spin states of Fe(III) ions limits their adsorption affinity. Herein, we develop a heteroatom-doping approach to boost the Cr(VI) removal efficacy of greigite. Compared to pristine greigite, cobalt doping significantly enhances the capability of greigite to adsorption Cr(VI) by decreasing electron occupancy in the eg orbitals and reducing the spin state of Fe ions. With a combination of electrochemical characterizations and theoretical calculations, we confirm that cobalt doping significantly enhances its reduction capacity toward Cr(VI) by elevating the d-band center and increasing electron transfer rate. We corroborate the finding by showing that Cu-doping, which has the opposite effects on d-orbital electron configures, compromises the efficacy of greigite. Of note, the magnetic properties of greigite remain largely unaffected upon heteroatom doping, allowing easy separation and recovery of the materials from the aqueous solutions. This work provides valuable mechanistic insights for nanomaterial design in contaminant removal and may inform the development of nanotechnology for green remediation of contaminated sites.
六价铬(Cr(VI))是地表水和地下水中经常检测到的受到最严格管制的污染物之一。磁性硫化铁是天然丰富的环保材料,是去除受污染水体中六价铬的理想材料,但是铁(III)离子的高自旋态限制了其吸附亲和力。在此,我们开发了一种杂原子掺杂方法来提高绿泥石去除六价铬的功效。与原始的绿泥石相比,钴掺杂通过降低eg轨道的电子占有率和铁离子的自旋态,显著增强了绿泥石吸附六价铬的能力。结合电化学特性分析和理论计算,我们证实掺钴可通过提高 d 带中心和增加电子转移率来显著增强对 Cr(VI) 的还原能力。我们还证实了这一发现,掺杂铜对 d-轨道电子构型的影响恰恰相反,会损害绿泥石的功效。值得注意的是,掺杂杂原子后,绿泥石的磁性能基本不受影响,因此很容易从水溶液中分离和回收材料。这项工作为污染物去除方面的纳米材料设计提供了宝贵的机理启示,并可为污染场地绿色修复纳米技术的开发提供参考。
{"title":"Modulating d-orbital electronic configuration of magnetic iron sulfide nanocrystals for maximized treatment efficiency of chromium-contaminated water","authors":"Yaqi Liu, Can Liu, Xiaofan Peng, Zongsheng Liang, Shengli Hou, Wei Chen, Tong Zhang","doi":"10.1016/j.watres.2025.123477","DOIUrl":"10.1016/j.watres.2025.123477","url":null,"abstract":"<div><div>Hexavalent chromium (Cr(VI)) is one of the most rigorously regulated contaminants frequently detected in surface and groundwater. Magnetic iron sulfides are naturally abundant, environmentally friendly materials ideal for the removal of Cr(VI) from contaminated water, but the high-spin states of Fe(III) ions limits their adsorption affinity. Herein, we develop a heteroatom-doping approach to boost the Cr(VI) removal efficacy of greigite. Compared to pristine greigite, cobalt doping significantly enhances the capability of greigite to adsorption Cr(VI) by decreasing electron occupancy in the <em>e<sub>g</sub></em> orbitals and reducing the spin state of Fe ions. With a combination of electrochemical characterizations and theoretical calculations, we confirm that cobalt doping significantly enhances its reduction capacity toward Cr(VI) by elevating the <em>d-</em>band center and increasing electron transfer rate. We corroborate the finding by showing that Cu-doping, which has the opposite effects on <em>d</em>-orbital electron configures, compromises the efficacy of greigite. Of note, the magnetic properties of greigite remain largely unaffected upon heteroatom doping, allowing easy separation and recovery of the materials from the aqueous solutions. This work provides valuable mechanistic insights for nanomaterial design in contaminant removal and may inform the development of nanotechnology for green remediation of contaminated sites.</div></div>","PeriodicalId":443,"journal":{"name":"Water Research","volume":"280 ","pages":"Article 123477"},"PeriodicalIF":11.4,"publicationDate":"2025-03-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143589952","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}