Water Research最新文献_第10页

Concurrent redox reactions for perfluorocarboxylic acids decontamination via UV-activated tryptophan/carbon nanotubes

IF 11.4 1区环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL

Water Research

Pub Date : 2025-03-13 DOI: 10.1016/j.watres.2025.123499

Han Wu , Jingquan Wang , Erdeng Du , Tao Liu , Min Liu , Hongguang Guo , Wenhai Chu

The contamination and persistence of Perfluorooctanoic Acid (PFOA) in aquatic environments have escalated environmental concerns, driving extensive research into effective decontamination strategies. To enhance the removal efficiency of PFOA via Advanced Reduction Processes (ARP) utilizing UV irradiation of tryptophan (Trp), carbon nanotubes (CNT) were incorporated, resulting in the development of a UV-Trp/CNT system. This novel process demonstrated a significant improvement in PFOA removal kinetics, as well as defluorination and Total Organic Carbon (TOC) reduction, and was effective across a broad spectrum of perfluoroalkyl carboxylic acids (PFCAs). In addition to the advanced reduction mechanism driven by hydrated electrons (

e_{a q}^{-}

), quenching experiments, material characterization, and chemical calculations indicated that CNTs facilitated the enrichment of Trp and PFOA, enabling electron transfer from PFOA to Trp via the CNT surface. This established a novel reaction pathway for PFOA oxidation coupled with ARP. The sequential defluorination of -CF₂- groups was facilitated by

e_{a q}^{-}

, while the electron transfer mechanism enabled oxidative decarboxylation, electron rearrangement, CC bond cleavage, and carbon chain shortening. These oxidative and reductive processes alternated systematically, advancing the development of a synergistic redox approach for the removal of PFCAs and inspiring further exploration into the use of carbon materials to construct confined domains and catalyze the degradation of PFASs.

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引用次数: 0

Crystalline phase regulates transformation and methylation of mercury sulfide nanoparticles in paddy systems

IF 11.4 1区环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL

Water Research

Pub Date : 2025-03-13 DOI: 10.1016/j.watres.2025.123496

Yunyun Li , Hong Li , Xujun Liang , Guoming Lin , Diandou Xu , Yuxi Gao , Lizhong Zhu , Jiating Zhao

Mercury sulfide nanoparticles (HgS_NPs) represent an important source of bioavailable mercury (Hg) for microbial methylation in paddy systems, depending on their size and crystalline phases. However, little is known about the phase compositions of HgS_NPs in Hg-contaminated paddy fields with dynamically changed redox conditions, their transformation, and methylation potential. Applying transmission electron microscopy (TEM) and synchrotron radiation X-ray absorption spectroscopy (SR-XAS), we found β-HgS_NPs as the predominant Hg species in newly contaminated areas, whereas α-HgS_NPs dominated in paddies near mining areas. Subsequent incubation assays indicated minimal phase transformation between α-HgS_NPs and β-HgS_NPs in simulated paddy systems, suggesting their high stability under natural conditions. Compared to α-HgS_NPs, β-HgS_NPs exhibited a higher methylation potential, as evidenced by greater production of methylmercury (MeHg) and elevated levels of Sn(II)-reducible Hg(II), a proxy for bioavailable Hg. Further experiments and density functional theory (DFT) calculations reveal that the higher bioavailability of β-HgS_NPs is closely linked to their crystalline phases and higher atomic binding energy for Hg²⁺ adsorption, as compared to α-HgS_NPs. This study, for the first time, unravels the significance of the crystalline phase in governing the bioavailability of HgS_NPs in paddy fields and provides novel insights into the ecological risk of HgS in wetland-like ecosystems.

{"title":"Crystalline phase regulates transformation and methylation of mercury sulfide nanoparticles in paddy systems","authors":"Yunyun Li , Hong Li , Xujun Liang , Guoming Lin , Diandou Xu , Yuxi Gao , Lizhong Zhu , Jiating Zhao","doi":"10.1016/j.watres.2025.123496","DOIUrl":"10.1016/j.watres.2025.123496","url":null,"abstract":"<div><div>Mercury sulfide nanoparticles (HgS<sub>NPs</sub>) represent an important source of bioavailable mercury (Hg) for microbial methylation in paddy systems, depending on their size and crystalline phases. However, little is known about the phase compositions of HgS<sub>NPs</sub> in Hg-contaminated paddy fields with dynamically changed redox conditions, their transformation, and methylation potential. Applying transmission electron microscopy (TEM) and synchrotron radiation X-ray absorption spectroscopy (SR-XAS), we found β-HgS<sub>NPs</sub> as the predominant Hg species in newly contaminated areas, whereas α-HgS<sub>NPs</sub> dominated in paddies near mining areas. Subsequent incubation assays indicated minimal phase transformation between α-HgS<sub>NPs</sub> and β-HgS<sub>NPs</sub> in simulated paddy systems, suggesting their high stability under natural conditions. Compared to α-HgS<sub>NPs</sub>, β-HgS<sub>NPs</sub> exhibited a higher methylation potential, as evidenced by greater production of methylmercury (MeHg) and elevated levels of Sn(II)-reducible Hg(II), a proxy for bioavailable Hg. Further experiments and density functional theory (DFT) calculations reveal that the higher bioavailability of β-HgS<sub>NPs</sub> is closely linked to their crystalline phases and higher atomic binding energy for Hg<sup>2+</sup> adsorption, as compared to α-HgS<sub>NPs</sub>. This study, for the first time, unravels the significance of the crystalline phase in governing the bioavailability of HgS<sub>NPs</sub> in paddy fields and provides novel insights into the ecological risk of HgS in wetland-like ecosystems.</div></div>","PeriodicalId":443,"journal":{"name":"Water Research","volume":"279 ","pages":"Article 123496"},"PeriodicalIF":11.4,"publicationDate":"2025-03-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143618579","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

DNA stable isotope probing and metagenomics reveal temperature responses of sulfur-driven autotrophic partial denitrification coupled with anammox (SPDA) system

IF 11.4 1区环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL

Water Research

Pub Date : 2025-03-13 DOI: 10.1016/j.watres.2025.123494

Qingteng Gong, Wei Zeng, Xiaojing Hao, Yifei Wang, Yongzhen Peng

The sulfur-driven autotrophic partial denitrification coupled with anammox (SPDA) process showed significant advantages in energy conservation and resource recovery in municipal wastewater treatment. However, its application in regions with seasonal temperature fluctuations and high latitudes is challenged by low temperatures. In this study, the feasibility of the SPDA process for treating low-strength municipal wastewater across a wide temperature range (30–10 °C) was systematically investigated. The results demonstrated that thiosulfate-driven autotrophic partial denitrification maintained an efficient nitrate removal rate of 7.82 mg NO₃^--N/gVSS/h and a nitrate to nitrite transformation rate of 62.7 % even at temperatures as low as 10 °C. Molecular ecological network and DNA-SIP revealed that dominant sulfur-oxidizing bacteria (SOB) shifted from norank_f_Hydrogenophilaceae and Thiobacillus at higher temperatures (30–20 °C) to Thiobacillus and Sulfurimonas as temperature decreased, thus ensuring the performance of autotrophic partial denitrification and consistent nitrite supply for anammox. Metagenomic analysis showed that the abundance of functional genes related to sulfur conversion increased almost universally, ensuring a stable electron supply for nitrate reduction through sulfur oxidation at low temperatures. The functional genes responsible for nitrate reduction changed from nar genes at higher temperatures to nap genes at lower temperatures, while a decrease in the abundance of hzs and hdh genes corresponding to reduced anammox performance. This study highlights the stable performance of the sulfur-driven autotrophic denitrification at low temperatures and the reliability of coupling with anammox, extending the applicability of SPDA to a broader geographical range.

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引用次数: 0

Comparative life cycle assessment of Fenton-like systems: Insights into the environmental benefits of reductant-driven strategies

IF 11.4 1区环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL

Water Research

Pub Date : 2025-03-13 DOI: 10.1016/j.watres.2025.123489

Daoyuan Zu , Jianbo Liu , Heting Wei , Kui Yang , Hailin Tian , Jinxing Ma , Zhifeng Yang

Reductant-driven Fenton-like advanced oxidation processes (AOPs) offer the potential to reduce transition metal and oxidant consumption, but the environmental implications of introducing reductants remain unclear. This study employs life cycle assessment (LCA) to evaluate the environmental impacts of reductant-driven Fenton-like systems as an alternative to conventional AOP. Five distinct Fenton-like systems were investigated, and their corresponding life cycle inventories compiled following systematic optimization of operating parameters. Results demonstrate that introducing reductant shifts environmental hotspots from oxidants to the added reductants. Commodity chemical reductants (hydroxylamine and ascorbic acid) significantly reduce energy consumption and environmental damage due to economies of scale. Their per unit Cumulative Energy Demand (CED) and environmental damage value are two orders of magnitude lower than those of specialty chemical reductants (10.31 and 8.93 MJ g⁻¹ MXene and MoS₂). Thus, novel catalysts, potentially associated with high energy consumption and toxic byproducts, require careful evaluation of their catalytic efficiency and unit environmental impact to determine overall environmental benefits. Scaling up chemical production, adopting regeneration strategy and transitioning to renewable energy sources represent key strategies for further environmental improvement. This study provides a quantitative framework for assessing the environmental performance of alternative Fenton-like systems, informing the design of more environmentally sustainable water purification technologies.

{"title":"Comparative life cycle assessment of Fenton-like systems: Insights into the environmental benefits of reductant-driven strategies","authors":"Daoyuan Zu , Jianbo Liu , Heting Wei , Kui Yang , Hailin Tian , Jinxing Ma , Zhifeng Yang","doi":"10.1016/j.watres.2025.123489","DOIUrl":"10.1016/j.watres.2025.123489","url":null,"abstract":"<div><div>Reductant-driven Fenton-like advanced oxidation processes (AOPs) offer the potential to reduce transition metal and oxidant consumption, but the environmental implications of introducing reductants remain unclear. This study employs life cycle assessment (LCA) to evaluate the environmental impacts of reductant-driven Fenton-like systems as an alternative to conventional AOP. Five distinct Fenton-like systems were investigated, and their corresponding life cycle inventories compiled following systematic optimization of operating parameters. Results demonstrate that introducing reductant shifts environmental hotspots from oxidants to the added reductants. Commodity chemical reductants (hydroxylamine and ascorbic acid) significantly reduce energy consumption and environmental damage due to economies of scale. Their per unit Cumulative Energy Demand (CED) and environmental damage value are two orders of magnitude lower than those of specialty chemical reductants (10.31 and 8.93 MJ g<sup>−1</sup> MXene and MoS<sub>2</sub>). Thus, novel catalysts, potentially associated with high energy consumption and toxic byproducts, require careful evaluation of their catalytic efficiency and unit environmental impact to determine overall environmental benefits. Scaling up chemical production, adopting regeneration strategy and transitioning to renewable energy sources represent key strategies for further environmental improvement. This study provides a quantitative framework for assessing the environmental performance of alternative Fenton-like systems, informing the design of more environmentally sustainable water purification technologies.</div></div>","PeriodicalId":443,"journal":{"name":"Water Research","volume":"279 ","pages":"Article 123489"},"PeriodicalIF":11.4,"publicationDate":"2025-03-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143608139","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

Carboxyl-free polyamide reverse osmosis membrane with sustainable anti-fouling performance in treating industrial coke wastewater

IF 11.4 1区环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL

Water Research

Pub Date : 2025-03-13 DOI: 10.1016/j.watres.2025.123495

Yongkai Xu, Shuang Hao, Dingxian Jia, Yiwen Qin, Jianxiao Wang, Jie Gao, Jun Xiao, Yunxia Hu

Carboxyl groups in polyamide (PA) reverse osmosis (RO) membrane contribute significantly to fouling and scaling, hindering the sustainable operation of RO in practical applications. Herein, we developed a novel interfacial polymerization (IP) strategy to finely engineer the molecular structure of PA with no carboxyl groups, and to significantly enhance RO membrane fouling/scaling-resistance. During IP, trimesoyl chloride (TMC) at the interface was consumed completely by the diffused m-phenylenediamine (MPD) and glycerol (GLY) under the assistance of benzalkonium chloride (BAC) surfactant. The fabricated RO membrane with no carboxyl groups exhibits sustainable anti-fouling performance with low flux decline ratios and high flux recovery ratios during the five cycles of fouling and cleaning when treating real coke wastewater, surpassing the reported anti-fouling membranes and the renowned commercial fouling-resistant RO membrane (DuPont FilmTec™ CR100). This work provides some insights to precisely tailor the molecular structure of PA RO membrane with sustainable anti-fouling performance.

{"title":"Carboxyl-free polyamide reverse osmosis membrane with sustainable anti-fouling performance in treating industrial coke wastewater","authors":"Yongkai Xu, Shuang Hao, Dingxian Jia, Yiwen Qin, Jianxiao Wang, Jie Gao, Jun Xiao, Yunxia Hu","doi":"10.1016/j.watres.2025.123495","DOIUrl":"10.1016/j.watres.2025.123495","url":null,"abstract":"<div><div>Carboxyl groups in polyamide (PA) reverse osmosis (RO) membrane contribute significantly to fouling and scaling, hindering the sustainable operation of RO in practical applications. Herein, we developed a novel interfacial polymerization (IP) strategy to finely engineer the molecular structure of PA with no carboxyl groups, and to significantly enhance RO membrane fouling/scaling-resistance. During IP, trimesoyl chloride (TMC) at the interface was consumed completely by the diffused m-phenylenediamine (MPD) and glycerol (GLY) under the assistance of benzalkonium chloride (BAC) surfactant. The fabricated RO membrane with no carboxyl groups exhibits sustainable anti-fouling performance with low flux decline ratios and high flux recovery ratios during the five cycles of fouling and cleaning when treating real coke wastewater, surpassing the reported anti-fouling membranes and the renowned commercial fouling-resistant RO membrane (DuPont FilmTec™ CR100). This work provides some insights to precisely tailor the molecular structure of PA RO membrane with sustainable anti-fouling performance.</div></div>","PeriodicalId":443,"journal":{"name":"Water Research","volume":"280 ","pages":"Article 123495"},"PeriodicalIF":11.4,"publicationDate":"2025-03-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143608140","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

Improved anaerobic digestion of waste activated sludge under ammonia stress by nanoscale zero-valent iron/peracetic acid pretreatment and hydrochar regulation: Insights from multi-omics analyses

IF 11.4 1区环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL

Water Research

Pub Date : 2025-03-13 DOI: 10.1016/j.watres.2025.123497

Qiya Sun , Dunjie Li , Yunpeng He , Qian Ping , Lin Wang , Yongmei Li

This study developed a novel strategy combining a nanoscale zero-valent iron (nZVI)/peracetic acid (PAA) pretreatment and hydrochar regulation to enhance anaerobic digestion of waste activated sludge (WAS) under ammonia-stressed conditions. The strategy significantly enhanced methane production at ammonia concentrations below 3000 mg/L, with the regulation groups (AN3000/REG) achieving a 50.1 % increase in cumulative methane yield. Metagenomic analysis demonstrated a 14.2 % enrichment of key functional microorganisms, including syntrophic fatty acid-oxidizing bacteria and hydrogenotrophic methanogens, in the AN3000/REG groups. Some of them promote the conversion of butyrate and valerate to acetate through the upregulation of key genes in the fatty acid β-oxidation pathway, thereby supplying sufficient substrates for acetoclastic methanogenesis. Beyond enhancing acetoclastic methanogenesis, the AN3000/REG groups exhibited significant upregulation of other metabolic pathways, with a 34.2 % increase in syntrophic acetate oxidation-hydrogenotrophic methanogenesis genes and a 17.1 % increase in methanol/methylotrophic methanogenesis-related genes. These findings were further validated by the metatranscriptomic and metaproteomic combination analyses. Furthermore, the AN3000/REG groups exhibited a significant enhancement in direct interspecies electron transfer, with functional microbes (e.g., Geobacter, Methanosarcina, and Methanobacterium), pili, and cytochrome c showing significant increases of 1.38-fold, 12.7-fold, and 5.6-fold, respectively. This might be due to the synergistic effects of nZVI and hydrochar in the regulation groups. Additionally, metabolomic analyses revealed that the regulation strategy improved the microbial adaptability to ammonia stress by modulating metabolic products, such as alkaloids. Our study not only provides a promising strategy for alleviating ammonia inhibition during the anaerobic digestion of WAS but also provides a strong basis for understanding the underlying mechanism under ammonia-stressed conditions.

{"title":"Improved anaerobic digestion of waste activated sludge under ammonia stress by nanoscale zero-valent iron/peracetic acid pretreatment and hydrochar regulation: Insights from multi-omics analyses","authors":"Qiya Sun , Dunjie Li , Yunpeng He , Qian Ping , Lin Wang , Yongmei Li","doi":"10.1016/j.watres.2025.123497","DOIUrl":"10.1016/j.watres.2025.123497","url":null,"abstract":"<div><div>This study developed a novel strategy combining a nanoscale zero-valent iron (nZVI)/peracetic acid (PAA) pretreatment and hydrochar regulation to enhance anaerobic digestion of waste activated sludge (WAS) under ammonia-stressed conditions. The strategy significantly enhanced methane production at ammonia concentrations below 3000 mg/L, with the regulation groups (AN3000/REG) achieving a 50.1 % increase in cumulative methane yield. Metagenomic analysis demonstrated a 14.2 % enrichment of key functional microorganisms, including syntrophic fatty acid-oxidizing bacteria and hydrogenotrophic methanogens, in the AN3000/REG groups. Some of them promote the conversion of butyrate and valerate to acetate through the upregulation of key genes in the fatty acid β-oxidation pathway, thereby supplying sufficient substrates for acetoclastic methanogenesis. Beyond enhancing acetoclastic methanogenesis, the AN3000/REG groups exhibited significant upregulation of other metabolic pathways, with a 34.2 % increase in syntrophic acetate oxidation-hydrogenotrophic methanogenesis genes and a 17.1 % increase in methanol/methylotrophic methanogenesis-related genes. These findings were further validated by the metatranscriptomic and metaproteomic combination analyses. Furthermore, the AN3000/REG groups exhibited a significant enhancement in direct interspecies electron transfer, with functional microbes (e.g., <em>Geobacter, Methanosarcina</em>, and <em>Methanobacterium</em>), pili, and cytochrome c showing significant increases of 1.38-fold, 12.7-fold, and 5.6-fold, respectively. This might be due to the synergistic effects of nZVI and hydrochar in the regulation groups. Additionally, metabolomic analyses revealed that the regulation strategy improved the microbial adaptability to ammonia stress by modulating metabolic products, such as alkaloids. Our study not only provides a promising strategy for alleviating ammonia inhibition during the anaerobic digestion of WAS but also provides a strong basis for understanding the underlying mechanism under ammonia-stressed conditions.</div></div>","PeriodicalId":443,"journal":{"name":"Water Research","volume":"279 ","pages":"Article 123497"},"PeriodicalIF":11.4,"publicationDate":"2025-03-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143618582","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

Explainable machine learning models enhance prediction of PFAS bioactivity using quantitative molecular surface analysis-derived representation

IF 11.4 1区环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL

Water Research

Pub Date : 2025-03-13 DOI: 10.1016/j.watres.2025.123500

Zhipeng Yin , Min Zhang , Runzeng Liu , Yong Cai

The extensive use of per- and polyfluoroalkyl substances (PFAS) in industrial and consumer products poses health risks due to their toxicity. Computational toxicology approaches, particularly quantitative structure-activity relationship (QSAR) models are essential for predicting PFAS bioactivity. However, established QSAR models including machine learning-based ones with traditional molecular descriptors such as constitutional, topological, and geometric descriptors, have limited predictive capability and interpretability. Herein, we proposed a novel machine learning approach that leverages quantitative molecular surface analysis (QMSA) of molecular electrostatic potential. Using QMSA descriptors, five machine learning models (e.g., random forest) achieved outstanding performance, with best accuracy of 0.950 ± 0.017, AUC-ROC of 0.938 ± 0.012, F1-score of 0.734 ± 0.024, and MCC of 0.684 ± 0.111 for five targets (tyrosyl-DNA phosphodiesterase 1 in the absence/presence of camptothecin, ATXN2 protein, transcription factor SMAD3, and transcription factor NRF2), which outperform previously reported models. SHAP analyses revealed that estimated density, molecular volume, positive surface area, and nonpolar surface area were the most important descriptors. These descriptors were deeply involved in PFAS binding to target proteins via non-covalent interactions as evidenced by molecular docking and molecular dynamics simulations. Our results demonstrated that QMSA descriptors-based machine learning models are capable of predicting PFAS toxicity with extraordinary performance and interpretability. This study provides a novel machine learning framework for the high-throughput and cost-effective screening of high-risk emerging PFAS in aquatic environments. By identifying the contaminants that should be prioritized for regulation and treatment among the growing number of PFAS, our work aids in water quality monitoring and risk assessment, and guides decision-making in aquatic environmental management. Furthermore, this work enhances our understanding of the molecular mechanisms involved in PFAS bioactivity.

{"title":"Explainable machine learning models enhance prediction of PFAS bioactivity using quantitative molecular surface analysis-derived representation","authors":"Zhipeng Yin , Min Zhang , Runzeng Liu , Yong Cai","doi":"10.1016/j.watres.2025.123500","DOIUrl":"10.1016/j.watres.2025.123500","url":null,"abstract":"<div><div>The extensive use of per- and polyfluoroalkyl substances (PFAS) in industrial and consumer products poses health risks due to their toxicity. Computational toxicology approaches, particularly quantitative structure-activity relationship (QSAR) models are essential for predicting PFAS bioactivity. However, established QSAR models including machine learning-based ones with traditional molecular descriptors such as constitutional, topological, and geometric descriptors, have limited predictive capability and interpretability. Herein, we proposed a novel machine learning approach that leverages quantitative molecular surface analysis (QMSA) of molecular electrostatic potential. Using QMSA descriptors, five machine learning models (e.g., random forest) achieved outstanding performance, with best accuracy of 0.950 ± 0.017, AUC-ROC of 0.938 ± 0.012, F1-score of 0.734 ± 0.024, and MCC of 0.684 ± 0.111 for five targets (tyrosyl-DNA phosphodiesterase 1 in the absence/presence of camptothecin, ATXN2 protein, transcription factor SMAD3, and transcription factor NRF2), which outperform previously reported models. SHAP analyses revealed that estimated density, molecular volume, positive surface area, and nonpolar surface area were the most important descriptors. These descriptors were deeply involved in PFAS binding to target proteins via non-covalent interactions as evidenced by molecular docking and molecular dynamics simulations. Our results demonstrated that QMSA descriptors-based machine learning models are capable of predicting PFAS toxicity with extraordinary performance and interpretability. This study provides a novel machine learning framework for the high-throughput and cost-effective screening of high-risk emerging PFAS in aquatic environments. By identifying the contaminants that should be prioritized for regulation and treatment among the growing number of PFAS, our work aids in water quality monitoring and risk assessment, and guides decision-making in aquatic environmental management. Furthermore, this work enhances our understanding of the molecular mechanisms involved in PFAS bioactivity.</div></div>","PeriodicalId":443,"journal":{"name":"Water Research","volume":"280 ","pages":"Article 123500"},"PeriodicalIF":11.4,"publicationDate":"2025-03-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143618577","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

Antibiotics shape the core microbial community distribution between floc and biofilm in an endogenous partial denitrification system: Insight from metabolic pathway

IF 11.4 1区环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL

Water Research

Pub Date : 2025-03-12 DOI: 10.1016/j.watres.2025.123491

Kai-Yue Dong, Chao-Xi Yang, Jin-Luo Pang, Rong-Rong Chang, Ke-Yu Chen, Wei Yao, Bao-Cheng Huang, Ren-Cun Jin

The response mechanism of microorganisms in partial denitrification (PD) system under antibiotic stress, particularly microbial energy metabolism and electron transfer, remain inadequately understood. This knowledge gap hinders the establishment of ecological links between microbial dynamics and macro-level reactor performance. To address this, moving bed biofilm reactors were employed to investigate the dynamic changes of microbial community and metabolism under sulfadiazine (SDZ) and ciprofloxacin (CIP) stress. Results showed that dosing 2 mg/L SDZ or CIP accelerated nitrite accumulation, achieving this milestone 15 days earlier than in the control group. At the end of the operational phase, nitrate removal efficiencies reached 90.3 ± 18.3 % (Control), 83.5 ± 16.2 % (SDZ-treated) and 93.9 ± 12.4 % (CIP-treated), with nitrate-to nitrite-transformation rates of 61.3 ± 12.7 %, 65.6 ± 13.1 % and 58.0 ± 21.2 %, respectively. The abundances of energy supply related genes, i.e., sucC and PK were higher in the CIP-treated group, while those in the other two groups were similar. The promoted tricarboxylic acid cycle and glycolysis led to NADH and ATP accumulation, accelerating nitrogen metabolism and benefiting early nitrite accumulation in the antibiotic-stressed system. More importantly, increasing antibiotics concentration from 2 mg/L to 4 mg/L induced selective migration of Thauera from floc to biofilm (abundance in floc reduced to < 2.01 %). Metagenomic sequencing indicated that the higher abundance of narGHI in biofilms, compared to flocs, was crucial for maintaining stable PD performance under antibiotic stress. The electron transport related genes, such as IDH1, DLD and DLAT, were more abundant in biofilms than in flocs after SDZ and CIP addition. These findings provide a theoretical basis for understanding the response mechanism of PD consortia to antibiotic.

{"title":"Antibiotics shape the core microbial community distribution between floc and biofilm in an endogenous partial denitrification system: Insight from metabolic pathway","authors":"Kai-Yue Dong, Chao-Xi Yang, Jin-Luo Pang, Rong-Rong Chang, Ke-Yu Chen, Wei Yao, Bao-Cheng Huang, Ren-Cun Jin","doi":"10.1016/j.watres.2025.123491","DOIUrl":"10.1016/j.watres.2025.123491","url":null,"abstract":"<div><div>The response mechanism of microorganisms in partial denitrification (PD) system under antibiotic stress, particularly microbial energy metabolism and electron transfer, remain inadequately understood. This knowledge gap hinders the establishment of ecological links between microbial dynamics and macro-level reactor performance. To address this, moving bed biofilm reactors were employed to investigate the dynamic changes of microbial community and metabolism under sulfadiazine (SDZ) and ciprofloxacin (CIP) stress. Results showed that dosing 2 mg/L SDZ or CIP accelerated nitrite accumulation, achieving this milestone 15 days earlier than in the control group. At the end of the operational phase, nitrate removal efficiencies reached 90.3 ± 18.3 % (Control), 83.5 ± 16.2 % (SDZ-treated) and 93.9 ± 12.4 % (CIP-treated), with nitrate-to nitrite-transformation rates of 61.3 ± 12.7 %, 65.6 ± 13.1 % and 58.0 ± 21.2 %, respectively. The abundances of energy supply related genes, i.e., <em>suc</em>C and <em>PK</em> were higher in the CIP-treated group, while those in the other two groups were similar. The promoted tricarboxylic acid cycle and glycolysis led to NADH and ATP accumulation, accelerating nitrogen metabolism and benefiting early nitrite accumulation in the antibiotic-stressed system. More importantly, increasing antibiotics concentration from 2 mg/L to 4 mg/L induced selective migration of <em>Thauera</em> from floc to biofilm (abundance in floc reduced to < 2.01 %). Metagenomic sequencing indicated that the higher abundance of <em>nar</em>GHI in biofilms, compared to flocs, was crucial for maintaining stable PD performance under antibiotic stress. The electron transport related genes, such as <em>IDH1, DLD</em> and <em>DLAT</em>, were more abundant in biofilms than in flocs after SDZ and CIP addition. These findings provide a theoretical basis for understanding the response mechanism of PD consortia to antibiotic.</div></div>","PeriodicalId":443,"journal":{"name":"Water Research","volume":"280 ","pages":"Article 123491"},"PeriodicalIF":11.4,"publicationDate":"2025-03-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143599415","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

Unveiling the directional dynamics: Hydrated electron driven defluorination in PFOA⁻ and PFOS⁻ through ab Initio molecular dynamics and quantum chemistry

IF 11.4 1区环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL

Water Research

Pub Date : 2025-03-12 DOI: 10.1016/j.watres.2025.123486

Chencheng Dai , Kaixin Li , Yazi Liu , BoChen Teng , Qi Chen , Xin Jin , Dayong Xu , Ran Hong

Hydrated electrons (e⁻(aq)) are recognized for their potent reducing capabilities, making them significant in environmental engineering, particularly in the degradation of persistent pollutants like perfluoroalkyl compounds (PFCs). This study investigates the influence of attack direction of e⁻(aq) on the degradation mechanisms of PFCs, addressing a critical gap in understanding due to experimental limitations. Utilizing ab initio molecular dynamics and quantum chemical calculations, we systematically simulated the attack direction of e⁻(aq) on PFCs, focusing on the formation of anionic radicals and their excited-state reactivity. Our results indicate that the attack direction is pivotal for C-F bond cleavage: e⁻(aq) targeting the carboxyl end promotes effective bond cleavage, while approaches from the carbon-fluorine chain are hindered by molecular orbital shielding effects. Furthermore, we demonstrate that employing micellar systems to maintain PFCs in an unsolvated anionic state significantly reduces excitation energy, enhances red-shifted absorption, and increases excitation probability. Importantly, the excited-state electronic structure of PFCs closely mirrors that of their anionic radicals. These findings provide a novel strategy for improving the degradation of PFCs, thereby advancing treatment processes for persistent environmental pollutants and contributing to the broader understanding of water quality management.

{"title":"Unveiling the directional dynamics: Hydrated electron driven defluorination in PFOA⁻ and PFOS⁻ through ab Initio molecular dynamics and quantum chemistry","authors":"Chencheng Dai , Kaixin Li , Yazi Liu , BoChen Teng , Qi Chen , Xin Jin , Dayong Xu , Ran Hong","doi":"10.1016/j.watres.2025.123486","DOIUrl":"10.1016/j.watres.2025.123486","url":null,"abstract":"<div><div>Hydrated electrons (<em>e</em><sup>−</sup>(<em>aq</em>)) are recognized for their potent reducing capabilities, making them significant in environmental engineering, particularly in the degradation of persistent pollutants like perfluoroalkyl compounds (PFCs). This study investigates the influence of attack direction of <em>e</em><sup>−</sup>(<em>aq</em>) on the degradation mechanisms of PFCs, addressing a critical gap in understanding due to experimental limitations. Utilizing <em>ab initio</em> molecular dynamics and quantum chemical calculations, we systematically simulated the attack direction of <em>e</em><sup>−</sup>(<em>aq</em>) on PFCs, focusing on the formation of anionic radicals and their excited-state reactivity. Our results indicate that the attack direction is pivotal for C-F bond cleavage: <em>e</em><sup>−</sup>(<em>aq</em>) targeting the carboxyl end promotes effective bond cleavage, while approaches from the carbon-fluorine chain are hindered by molecular orbital shielding effects. Furthermore, we demonstrate that employing micellar systems to maintain PFCs in an unsolvated anionic state significantly reduces excitation energy, enhances red-shifted absorption, and increases excitation probability. Importantly, the excited-state electronic structure of PFCs closely mirrors that of their anionic radicals. These findings provide a novel strategy for improving the degradation of PFCs, thereby advancing treatment processes for persistent environmental pollutants and contributing to the broader understanding of water quality management.</div></div>","PeriodicalId":443,"journal":{"name":"Water Research","volume":"280 ","pages":"Article 123486"},"PeriodicalIF":11.4,"publicationDate":"2025-03-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143608195","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

Selective activation of peroxymonosulfate through gating heteronuclear diatomic distance for flexible generation of high-valent cobalt-oxo species or sulfate radicals

IF 11.4 1区环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL

Water Research

Pub Date : 2025-03-12 DOI: 10.1016/j.watres.2025.123488

Jingjing Jiang , Yanan Zhang , Yansong Liu , Shengda Liu , Tongze Sun , Bowen Zhao , Ruixin Wang , Chongjun Zhang , Mingxin Huo , Dandan Zhou , Shuangshi Dong

Heteronuclear diatomic engineering has been widely applied to generate selective or nonselective active species in Fenton-like system for wastewater treatment. However, active species adapted to diverse wastewater were different, and flexible control of active species has remained elusive, often necessitating complex and repetitive atom modifications. Here, we proposed a diatomic distance gating strategy that adjusted the spintronic structure of cobalt site for flexible transformation of high-valent cobalt-oxo and sulfate radical for adapted wastewater treatment. Electron paramagnetic resonance spectra, magnetic susceptibility-temperatur curve and partial density of states revealed electron transfer from dx²−y², dz² and dyz orbitals of high-spin cobalt to peroxymonosulfate for high-valent cobalt-oxo generation at 3.8 nm, and from dz² orbital of medium-spin cobalt to peroxymonosulfate for sulfate radical generation at 2.5 nm. The Fenton-like system with 3.8 nm of diatomic distance preferentially degraded contaminants with low n-octanol/water partition constant and high ionization potential, while Fenton-like system with 2.5 nm of diatomic distance readily degraded contaminants with high Hammett substituent constant and low dissociation constant. This study elucidated the effect of diatomic distance on Fenton-like chemistry and provided a blueprint for the design of intelligent Fenton-like system for treating diverse wastewater treatment scenarios.

{"title":"Selective activation of peroxymonosulfate through gating heteronuclear diatomic distance for flexible generation of high-valent cobalt-oxo species or sulfate radicals","authors":"Jingjing Jiang , Yanan Zhang , Yansong Liu , Shengda Liu , Tongze Sun , Bowen Zhao , Ruixin Wang , Chongjun Zhang , Mingxin Huo , Dandan Zhou , Shuangshi Dong","doi":"10.1016/j.watres.2025.123488","DOIUrl":"10.1016/j.watres.2025.123488","url":null,"abstract":"<div><div>Heteronuclear diatomic engineering has been widely applied to generate selective or nonselective active species in Fenton-like system for wastewater treatment. However, active species adapted to diverse wastewater were different, and flexible control of active species has remained elusive, often necessitating complex and repetitive atom modifications. Here, we proposed a diatomic distance gating strategy that adjusted the spintronic structure of cobalt site for flexible transformation of high-valent cobalt-oxo and sulfate radical for adapted wastewater treatment. Electron paramagnetic resonance spectra, magnetic susceptibility-temperatur curve and partial density of states revealed electron transfer from <em>dx<sup>2</sup>−y<sup>2</sup>, dz<sup>2</sup></em> and <em>dyz</em> orbitals of high-spin cobalt to peroxymonosulfate for high-valent cobalt-oxo generation at 3.8 nm, and from <em>dz<sup>2</sup></em> orbital of medium-spin cobalt to peroxymonosulfate for sulfate radical generation at 2.5 nm. The Fenton-like system with 3.8 nm of diatomic distance preferentially degraded contaminants with low n-octanol/water partition constant and high ionization potential, while Fenton-like system with 2.5 nm of diatomic distance readily degraded contaminants with high Hammett substituent constant and low dissociation constant. This study elucidated the effect of diatomic distance on Fenton-like chemistry and provided a blueprint for the design of intelligent Fenton-like system for treating diverse wastewater treatment scenarios.</div></div>","PeriodicalId":443,"journal":{"name":"Water Research","volume":"279 ","pages":"Article 123488"},"PeriodicalIF":11.4,"publicationDate":"2025-03-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143599128","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