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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
Biological methane removal by groundwater trickling biofiltration for emissions reduction
IF 11.4 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2025-03-06 DOI: 10.1016/j.watres.2025.123450
Francesc Corbera-Rubio , Alje S. Boersma , Weren de Vet , Martin Pabst , Paul W.J.J. van der Wielen , Maartje A.H.J. van Kessel , Mark C.M. van Loosdrecht , Doris van Halem , Sebastian Lücker , Michele Laureni
Methane removal is an essential step in drinking water production from methane-rich groundwaters. Conventional aeration-based stripping results in significant direct methane emissions, contributing up to one-third of a treatment plant's total carbon footprint. To address this, a full-scale trickling filter was operated for biological methane oxidation upstream of a submerged sand filter, and its performance was compared to a conventional aeration–submerged sand filtration set-up. Full-scale data were combined with ex-situ batch assays and metagenome-resolved metaproteomics to quantify the individual contribution of the main (a)biotic processes and characterize the enriched microbial communities. Both treatment setups fully removed methane, iron, ammonium, and manganese, yet the underlying mechanisms differed significantly. Methane was completely removed from the effluent after trickling filtration, with stripping and biological oxidation each accounting for half of the removal, thereby halving overall methane emissions. Methane-oxidizing bacteria not only outcompeted nitrifiers in the trickling filter, but also likely contributed directly to ammonia oxidation. In contrast to the submerged filter preceded by methane stripping, signatures of biological iron oxidation were almost completely absent in the trickling filter, suggesting that the presence of methane directly or indirectly promotes chemical iron oxidation. All systems had similar ex-situ manganese oxidation capacities, yet removal occurred only in the submerged filters but not the trickling filter. Ultimately, our results demonstrate that trickling filtration is effective in promoting biological methane oxidation at comparable produced drinking water quality, highlighting its potential for advancing sustainable drinking water production.
{"title":"Biological methane removal by groundwater trickling biofiltration for emissions reduction","authors":"Francesc Corbera-Rubio ,&nbsp;Alje S. Boersma ,&nbsp;Weren de Vet ,&nbsp;Martin Pabst ,&nbsp;Paul W.J.J. van der Wielen ,&nbsp;Maartje A.H.J. van Kessel ,&nbsp;Mark C.M. van Loosdrecht ,&nbsp;Doris van Halem ,&nbsp;Sebastian Lücker ,&nbsp;Michele Laureni","doi":"10.1016/j.watres.2025.123450","DOIUrl":"10.1016/j.watres.2025.123450","url":null,"abstract":"<div><div>Methane removal is an essential step in drinking water production from methane-rich groundwaters. Conventional aeration-based stripping results in significant direct methane emissions, contributing up to one-third of a treatment plant's total carbon footprint. To address this, a full-scale trickling filter was operated for biological methane oxidation upstream of a submerged sand filter, and its performance was compared to a conventional aeration–submerged sand filtration set-up. Full-scale data were combined with <em>ex-situ</em> batch assays and metagenome-resolved metaproteomics to quantify the individual contribution of the main (a)biotic processes and characterize the enriched microbial communities. Both treatment setups fully removed methane, iron, ammonium, and manganese, yet the underlying mechanisms differed significantly. Methane was completely removed from the effluent after trickling filtration, with stripping and biological oxidation each accounting for half of the removal, thereby halving overall methane emissions. Methane-oxidizing bacteria not only outcompeted nitrifiers in the trickling filter, but also likely contributed directly to ammonia oxidation. In contrast to the submerged filter preceded by methane stripping, signatures of biological iron oxidation were almost completely absent in the trickling filter, suggesting that the presence of methane directly or indirectly promotes chemical iron oxidation. All systems had similar <em>ex-situ</em> manganese oxidation capacities, yet removal occurred only in the submerged filters but not the trickling filter. Ultimately, our results demonstrate that trickling filtration is effective in promoting biological methane oxidation at comparable produced drinking water quality, highlighting its potential for advancing sustainable drinking water production.</div></div>","PeriodicalId":443,"journal":{"name":"Water Research","volume":"279 ","pages":"Article 123450"},"PeriodicalIF":11.4,"publicationDate":"2025-03-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143570096","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
Exacerbated anthropogenic water pollution under climate change and urbanization
IF 11.4 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2025-03-06 DOI: 10.1016/j.watres.2025.123449
Wenyu Yang , Christian Schmidt , Shixue Wu , Ziyong Zhao , Ruifei Li , Zhenyu Wang , Haijun Wang , Pei Hua , Peter Krebs , Jin Zhang
Anthropogenic water pollution severely threatens human society worldwide, yet the water pollution induced by combined sewer overflow (CSO) remains unclear within climate change and urbanization. Hence, this study integrated the general circulation model (GCM) and shared socioeconomic pathway (SSP) projections with water quality modeling, to analyze spatiotemporal patterns and future trends of CSO-induced water pollution under changing environments. Results demonstrated that the given area (Dresden, Germany) encountered significant CSO-induced pollution, with 14,860 kg (95 % confidence interval, CI: 9,040–15,630 kg) of particulate matter (SS), organic compounds (COD, TN, TP), and pharmaceuticals (Carbamazepine, Gabapentin, Ciprofloxacin, Sulfamethoxazole) being discharged annually. Climate change and urbanization exacerbated the severity of CSO-induced pollution, causing the discharged pollutants to reach a maximum annual load of 34,900 kg (CI: 21,400–44,100 kg), with up to 82.19 % of organic compounds and 75.28 % of pharmaceuticals being discharged by the top 25 % of extreme CSOs. GIS-based spatial analysis indicated the regional heterogeneities of CSO-induced pollution, the high-frequency CSOs were predominantly located in highly-impervious areas, while the high-load discharges mainly occurred in densely-populated areas. Scenario analysis revealed stronger temporal variabilities of CSO-induced pollution in the future, with the seasonal anomalies of discharged loads ranging from -86.18 % to 76.89 %. In addition, pharmaceutical pollution exhibited significant uncertainties under changing environments, and the CI of discharged load expanded by up to 131.71 %. The methods and findings herein yielded further insights into water quality management in response to changing environments.
{"title":"Exacerbated anthropogenic water pollution under climate change and urbanization","authors":"Wenyu Yang ,&nbsp;Christian Schmidt ,&nbsp;Shixue Wu ,&nbsp;Ziyong Zhao ,&nbsp;Ruifei Li ,&nbsp;Zhenyu Wang ,&nbsp;Haijun Wang ,&nbsp;Pei Hua ,&nbsp;Peter Krebs ,&nbsp;Jin Zhang","doi":"10.1016/j.watres.2025.123449","DOIUrl":"10.1016/j.watres.2025.123449","url":null,"abstract":"<div><div>Anthropogenic water pollution severely threatens human society worldwide, yet the water pollution induced by combined sewer overflow (CSO) remains unclear within climate change and urbanization. Hence, this study integrated the general circulation model (GCM) and shared socioeconomic pathway (SSP) projections with water quality modeling, to analyze spatiotemporal patterns and future trends of CSO-induced water pollution under changing environments. Results demonstrated that the given area (Dresden, Germany) encountered significant CSO-induced pollution, with 14,860 kg (95 % confidence interval, CI: 9,040–15,630 kg) of particulate matter (SS), organic compounds (COD, TN, TP), and pharmaceuticals (Carbamazepine, Gabapentin, Ciprofloxacin, Sulfamethoxazole) being discharged annually. Climate change and urbanization exacerbated the severity of CSO-induced pollution, causing the discharged pollutants to reach a maximum annual load of 34,900 kg (CI: 21,400–44,100 kg), with up to 82.19 % of organic compounds and 75.28 % of pharmaceuticals being discharged by the top 25 % of extreme CSOs. GIS-based spatial analysis indicated the regional heterogeneities of CSO-induced pollution, the high-frequency CSOs were predominantly located in highly-impervious areas, while the high-load discharges mainly occurred in densely-populated areas. Scenario analysis revealed stronger temporal variabilities of CSO-induced pollution in the future, with the seasonal anomalies of discharged loads ranging from -86.18 % to 76.89 %. In addition, pharmaceutical pollution exhibited significant uncertainties under changing environments, and the CI of discharged load expanded by up to 131.71 %. The methods and findings herein yielded further insights into water quality management in response to changing environments.</div></div>","PeriodicalId":443,"journal":{"name":"Water Research","volume":"280 ","pages":"Article 123449"},"PeriodicalIF":11.4,"publicationDate":"2025-03-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143570097","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
Diversity, influential factor, and communication network construction of quorum sensing bacteria in global wastewater treatment plants
IF 11.4 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2025-03-06 DOI: 10.1016/j.watres.2025.123437
Yong-Chao Wang , Sen Wang , Ya-Hui Lv , Jia-Yi Wang , Wen-Xuan Yang , Ye Deng , Feng Ju , Can Wang
Quorum sensing (QS) is widespread in the microbial world and mediates microbial relationships in communities. However, the existing knowledge is far from a full description of the complex communication-based microbial interactions in engineered ecosystems, i.e., wastewater treatment plants (WWTPs). Herein, we conducted a systematic analysis of the diversity and influential factors of the QS-related microflora through the collection of global 1186 activated sludge microbiome samples. We found that the richness of bacteria associated with the universal bacterial secondary messenger presented the highest in QS system, whereas the bacteria related to the degradation of N-Acyl-homoserine lactones occupied the main position in the quorum quenching system. The community turnover of QS microflora was found more likely to be dominated by the deterministic process, such as the dissolved oxygen and resource availability (the ratio of organic matter to microorganisms). Meanwhile, these QS microflora in turn have a profound impact on the functions of WWTPs, especially multilingual intelligencers involving various language systems, such as Nitrospira. By connecting the signal molecule synthesis and acceptance bacteria, we constructed a QS communication network, which can be a robust tool for initial investigation of signaling molecule-mediated microbial interactions. The above results were further integrated into an online access website, named Quorum Sensing Communication Network in Activated Sludge (QSCNAS) (https://www.qscnas.cn/), which allowed users to browse and capture possible QS-based interactions of target bacterium. This work contributes to the understanding of bacterial communication in WWTPs and provides a platform to help in developing potential regulation strategies.
{"title":"Diversity, influential factor, and communication network construction of quorum sensing bacteria in global wastewater treatment plants","authors":"Yong-Chao Wang ,&nbsp;Sen Wang ,&nbsp;Ya-Hui Lv ,&nbsp;Jia-Yi Wang ,&nbsp;Wen-Xuan Yang ,&nbsp;Ye Deng ,&nbsp;Feng Ju ,&nbsp;Can Wang","doi":"10.1016/j.watres.2025.123437","DOIUrl":"10.1016/j.watres.2025.123437","url":null,"abstract":"<div><div>Quorum sensing (QS) is widespread in the microbial world and mediates microbial relationships in communities. However, the existing knowledge is far from a full description of the complex communication-based microbial interactions in engineered ecosystems, i.e., wastewater treatment plants (WWTPs). Herein, we conducted a systematic analysis of the diversity and influential factors of the QS-related microflora through the collection of global 1186 activated sludge microbiome samples. We found that the richness of bacteria associated with the universal bacterial secondary messenger presented the highest in QS system, whereas the bacteria related to the degradation of <em>N</em>-Acyl-homoserine lactones occupied the main position in the quorum quenching system. The community turnover of QS microflora was found more likely to be dominated by the deterministic process, such as the dissolved oxygen and resource availability (the ratio of organic matter to microorganisms). Meanwhile, these QS microflora in turn have a profound impact on the functions of WWTPs, especially multilingual intelligencers involving various language systems, such as <em>Nitrospira</em>. By connecting the signal molecule synthesis and acceptance bacteria, we constructed a QS communication network, which can be a robust tool for initial investigation of signaling molecule-mediated microbial interactions. The above results were further integrated into an online access website, named Quorum Sensing Communication Network in Activated Sludge (QSCNAS) (<span><span>https://www.qscnas.cn/</span><svg><path></path></svg></span>), which allowed users to browse and capture possible QS-based interactions of target bacterium. This work contributes to the understanding of bacterial communication in WWTPs and provides a platform to help in developing potential regulation strategies.</div></div>","PeriodicalId":443,"journal":{"name":"Water Research","volume":"279 ","pages":"Article 123437"},"PeriodicalIF":11.4,"publicationDate":"2025-03-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143550522","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
Efficient antibiotic tetracycline degradation and toxicity abatement via the perovskite-type CaFexNi1-xO3 assisted heterogeneous electro-Fenton system
IF 11.4 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2025-03-06 DOI: 10.1016/j.watres.2025.123432
Yuling Liang , Aochen Feng , Naif Abdullah Al-Dhabi , Jing Zhang , Wenle Xing , Tao Chen , Yuxuan Han , Guangming Zeng , Lin Tang , Wangwang Tang
As one of the emerging contaminants, antibiotics are posing a great threat to the human health and environment, which requires effective treatment methods. Heterogeneous electro-Fenton is a promising technique for organic contaminant elimination, but preparation of an appropriate heterogeneous electro-Fenton catalyst still remains challenging. In this work, the feasibility of perovskite-type CaFexNi1-xO3 as heterogeneous electro-Fenton catalyst for tetracycline (TC) removal and toxicity abatement has been explored. It was found that, among the examined CaFexNi1-xO3 catalysts with different Ni doping amount, CaFe3/4Ni1/4O3 exhibited the best performance, achieving 92.1 % TC removal within 30 min without pH adjustment in the presence of 0.05 M Na2SO4 electrolyte. Choosing Cl-containing electrolyte enabled further improvement towards TC elimination. In addition, the CaFe3/4Ni1/4O3 based heterogeneous electro-Fenton system presented other advantages including good recyclability and universal applicability, and significant toxicity reduction (verified via both ECOSAR simulation and soybean germination test). The TC degradation pathways were elucidated through identification of intermediate products and DFT calculations. Mechanism investigations revealed that there existed a strong synergy between Fe and Ni, and ·OH and ·O2 played the primary roles in the system while 1O2 played an auxiliary role. This study presented a promising heterogeneous electro-Fenton catalyst for degradation of antibiotics such as tetracycline.
{"title":"Efficient antibiotic tetracycline degradation and toxicity abatement via the perovskite-type CaFexNi1-xO3 assisted heterogeneous electro-Fenton system","authors":"Yuling Liang ,&nbsp;Aochen Feng ,&nbsp;Naif Abdullah Al-Dhabi ,&nbsp;Jing Zhang ,&nbsp;Wenle Xing ,&nbsp;Tao Chen ,&nbsp;Yuxuan Han ,&nbsp;Guangming Zeng ,&nbsp;Lin Tang ,&nbsp;Wangwang Tang","doi":"10.1016/j.watres.2025.123432","DOIUrl":"10.1016/j.watres.2025.123432","url":null,"abstract":"<div><div>As one of the emerging contaminants, antibiotics are posing a great threat to the human health and environment, which requires effective treatment methods. Heterogeneous electro-Fenton is a promising technique for organic contaminant elimination, but preparation of an appropriate heterogeneous electro-Fenton catalyst still remains challenging. In this work, the feasibility of perovskite-type CaFe<sub>x</sub>Ni<sub>1-x</sub>O<sub>3</sub> as heterogeneous electro-Fenton catalyst for tetracycline (TC) removal and toxicity abatement has been explored. It was found that, among the examined CaFe<sub>x</sub>Ni<sub>1-x</sub>O<sub>3</sub> catalysts with different Ni doping amount, CaFe<sub>3/4</sub>Ni<sub>1/4</sub>O<sub>3</sub> exhibited the best performance, achieving 92.1 % TC removal within 30 min without pH adjustment in the presence of 0.05 M Na<sub>2</sub>SO<sub>4</sub> electrolyte. Choosing Cl<sup>−</sup>-containing electrolyte enabled further improvement towards TC elimination. In addition, the CaFe<sub>3/4</sub>Ni<sub>1/4</sub>O<sub>3</sub> based heterogeneous electro-Fenton system presented other advantages including good recyclability and universal applicability, and significant toxicity reduction (verified via both ECOSAR simulation and soybean germination test). The TC degradation pathways were elucidated through identification of intermediate products and DFT calculations. Mechanism investigations revealed that there existed a strong synergy between Fe and Ni, and ·OH and ·O<sub>2</sub><sup>−</sup> played the primary roles in the system while <sup>1</sup>O<sub>2</sub> played an auxiliary role. This study presented a promising heterogeneous electro-Fenton catalyst for degradation of antibiotics such as tetracycline.</div></div>","PeriodicalId":443,"journal":{"name":"Water Research","volume":"279 ","pages":"Article 123432"},"PeriodicalIF":11.4,"publicationDate":"2025-03-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143550658","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
The bidirectional matter transfer in adsorption-promoted photocatalytic ozonation system derived by triazine nanosheets-heptazine nanotubes homojunction composite biochar
IF 11.4 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2025-03-06 DOI: 10.1016/j.watres.2025.123444
Benjie Zhu , Jialiang Liu , Yuxiang Shen , Lingyu Liu , Fang Liu
Heterogeneous catalytic ozonation (HCO) process is an efficiency and eco-friendly solution to the growing challenge of water purification, yet is challenging by O3 utilization, pollutants selectivity, and matter transfer resistance. Herein, adsorption-promoted photocatalytic ozonation (HCO/POAP) system was constructed derived by triazine nanosheets-heptazine nanotubes homojunction carbon nitride composite Enteromorpha prolifera derived biochar (CNTh-St/EpC) to provide a targeted solution for the refractory organic pollutants treatment. In the HCO/POAP system, the adsorption sites predominantly reside on EpC, while the catalytic sites are primarily located on CN. The construction of efficient transport channels is facilitated by the induction of triazine structures from amorphous C, N compounds along the edges of heptazine. This leads to the independent yet closely interconnected process of inward transfer of pollutants and outward transfer of active species, confining reactions to a bidirectional transfer channel. This strategic confinement significantly amplifies the performance of HCO/POAP system. Specifically, the removal rates are 80 % for TC and 94 % for PNP in 30 min with almost entirely harmless or non-toxic degradation products, and mark a 56 % and 77 % enhancement over O3 system, respectively. Moreover, the HCO/POAP system demonstrates exceptional efficacy in treating dissolved organic matter, chemical oxygen demand (COD), and ultraviolet absorbance at 254 nm (UV254) in diverse actual wastewater. This study highlights the potential of HCO/POAP process in efficient water purification, and provides mechanistic insights into the bidirectional matter transfer during the contaminants remove.
{"title":"The bidirectional matter transfer in adsorption-promoted photocatalytic ozonation system derived by triazine nanosheets-heptazine nanotubes homojunction composite biochar","authors":"Benjie Zhu ,&nbsp;Jialiang Liu ,&nbsp;Yuxiang Shen ,&nbsp;Lingyu Liu ,&nbsp;Fang Liu","doi":"10.1016/j.watres.2025.123444","DOIUrl":"10.1016/j.watres.2025.123444","url":null,"abstract":"<div><div>Heterogeneous catalytic ozonation (HCO) process is an efficiency and eco-friendly solution to the growing challenge of water purification, yet is challenging by O<sub>3</sub> utilization, pollutants selectivity, and matter transfer resistance. Herein, adsorption-promoted photocatalytic ozonation (HCO/PO<sub>AP</sub>) system was constructed derived by triazine nanosheets-heptazine nanotubes homojunction carbon nitride composite Enteromorpha prolifera derived biochar (CN<sub>Th-St</sub>/EpC) to provide a targeted solution for the refractory organic pollutants treatment. In the HCO/PO<sub>AP</sub> system, the adsorption sites predominantly reside on EpC, while the catalytic sites are primarily located on CN. The construction of efficient transport channels is facilitated by the induction of triazine structures from amorphous C, N compounds along the edges of heptazine. This leads to the independent yet closely interconnected process of inward transfer of pollutants and outward transfer of active species, confining reactions to a bidirectional transfer channel. This strategic confinement significantly amplifies the performance of HCO/PO<sub>AP</sub> system. Specifically, the removal rates are 80 % for TC and 94 % for PNP in 30 min with almost entirely harmless or non-toxic degradation products, and mark a 56 % and 77 % enhancement over O<sub>3</sub> system, respectively. Moreover, the HCO/PO<sub>AP</sub> system demonstrates exceptional efficacy in treating dissolved organic matter, chemical oxygen demand (COD), and ultraviolet absorbance at 254 nm (UV<sub>254</sub>) in diverse actual wastewater. This study highlights the potential of HCO/PO<sub>AP</sub> process in efficient water purification, and provides mechanistic insights into the bidirectional matter transfer during the contaminants remove.</div></div>","PeriodicalId":443,"journal":{"name":"Water Research","volume":"279 ","pages":"Article 123444"},"PeriodicalIF":11.4,"publicationDate":"2025-03-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143570095","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
Insights into in-situ free nitrous acid induced extracellular polymeric substances changes and membrane fouling mitigation in a nitritation membrane bioreactor
IF 11.4 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2025-03-05 DOI: 10.1016/j.watres.2025.123446
Yishuai Jiang , Xiaoyuan Zhang , Hiroshige Shiota , Wun Jern Ng
This study investigated the effectiveness of free nitrous acid (FNA) on mitigating membrane fouling, with the associated mechanisms, in two nitritation membrane bioreactors (MBRs) operated with Nitrosomonas-enriched culture. Results showed that FNA stress, regulated by pH and nitrite concentration, maintained a low-level fouling as opposed to the control MBR where trans-membrane pressure (TMP) exceeded 30 kPa. Compared to the control MBR, production of biofilm in the FNA stressed MBR was reduced by 68.1% in terms of mass and 78.2% in terms of thickness. Suspended biomass and biofilm extracellular polymeric substances (EPS) characterized by liquid chromatography (LC-OCD-OND) indicated FNA stress reduced the amount of low molecular weight neutrals and hydrophobic dissolved organic carbon. These components would have had high fouling potential. Excitation emission matrix (EEM) fluorescence contours indicated that exposure to FNA stimulated the production of tyrosine-like proteins but reduced those of SMP like and humic acid-like substances. This could have affected the adhesion between bacteria and membrane and so contributed to the reduced biofilm and fouling. X-ray photoelectron spectroscopy (XPS) analysis revealed marked differences in intensities of the main functionalities in the EPS for both sludge and biofilm, due to the oxidative effect of FNA, e.g. FNA stress resulted in more aliphatic C-OH, amines and amides while the control had more C=O, amino acids and amino sugars. This study showed that in-situ generated FNA could be employed to mitigate membrane fouling effectively via its biocidal and oxidative effect.
{"title":"Insights into in-situ free nitrous acid induced extracellular polymeric substances changes and membrane fouling mitigation in a nitritation membrane bioreactor","authors":"Yishuai Jiang ,&nbsp;Xiaoyuan Zhang ,&nbsp;Hiroshige Shiota ,&nbsp;Wun Jern Ng","doi":"10.1016/j.watres.2025.123446","DOIUrl":"10.1016/j.watres.2025.123446","url":null,"abstract":"<div><div>This study investigated the effectiveness of free nitrous acid (FNA) on mitigating membrane fouling, with the associated mechanisms, in two nitritation membrane bioreactors (MBRs) operated with <em>Nitrosomonas-</em>enriched culture. Results showed that FNA stress, regulated by pH and nitrite concentration, maintained a low-level fouling as opposed to the control MBR where trans-membrane pressure (TMP) exceeded 30 kPa. Compared to the control MBR, production of biofilm in the FNA stressed MBR was reduced by 68.1% in terms of mass and 78.2% in terms of thickness. Suspended biomass and biofilm extracellular polymeric substances (EPS) characterized by liquid chromatography (LC-OCD-OND) indicated FNA stress reduced the amount of low molecular weight neutrals and hydrophobic dissolved organic carbon. These components would have had high fouling potential. Excitation emission matrix (EEM) fluorescence contours indicated that exposure to FNA stimulated the production of tyrosine-like proteins but reduced those of SMP like and humic acid-like substances. This could have affected the adhesion between bacteria and membrane and so contributed to the reduced biofilm and fouling. X-ray photoelectron spectroscopy (XPS) analysis revealed marked differences in intensities of the main functionalities in the EPS for both sludge and biofilm, due to the oxidative effect of FNA, e.g. FNA stress resulted in more aliphatic C-OH, amines and amides while the control had more C=O, amino acids and amino sugars. This study showed that <em>in-situ</em> generated FNA could be employed to mitigate membrane fouling effectively via its biocidal and oxidative effect.</div></div>","PeriodicalId":443,"journal":{"name":"Water Research","volume":"279 ","pages":"Article 123446"},"PeriodicalIF":11.4,"publicationDate":"2025-03-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143560880","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
Aging behaviors intensify the impacts of microplastics on nitrate bioreduction-driven nitrogen cycling in freshwater sediments
IF 11.4 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2025-03-05 DOI: 10.1016/j.watres.2025.123448
Yuecheng She , Liying Wu , Xin Qi , Siyu Sun , Zhengkui Li
Microplastics (MPs) inevitably undergo aging processes in natural environments; however, how aging behaviors influence the interactions between MPs exposures and nitrate bioreduction in freshwater sediments remains poorly understood. Here, we explored the distinct impacts of virgin and aged MPs (polystyrene (PS) and polylactic acid (PLA)) on nitrate bioreduction processes in lake sediments through a long-term microcosm experiment utilizing the 15N isotope tracing technique and molecular analysis. Compared to virgin MPs, aged PLA significantly increased the rates of denitrification, anaerobic ammonium oxidation (anammox), and dissimilatory nitrate reduction to ammonium (DNRA) (p < 0.05), facilitating sediment nitrogen loss, while aged PS only significantly improved the rates of DNRA by 272–297 % and contributed to nitrogen retention in sediments. Metagenomic sequencing demonstrated that a more significant enrichment of functional genes responsible for nitrate bioreduction pathways occurred with aged MPs exposures than with virgin MPs. By combining analyses of MPs aging traits and the key drivers of nitrate bioreduction, we revealed that aging behaviors directly regulated sediment nutrient status (e.g., DOC/NOx ratio) and microbiological properties (from genes to bacteria), thereby further determining the activity of nitrate bioreduction. This work provides new insights into the impacts of aged MPs on sediment nitrate reduction and highlights the role of MPs aging in future assessments of long-term MPs pollution in freshwater ecosystems.
{"title":"Aging behaviors intensify the impacts of microplastics on nitrate bioreduction-driven nitrogen cycling in freshwater sediments","authors":"Yuecheng She ,&nbsp;Liying Wu ,&nbsp;Xin Qi ,&nbsp;Siyu Sun ,&nbsp;Zhengkui Li","doi":"10.1016/j.watres.2025.123448","DOIUrl":"10.1016/j.watres.2025.123448","url":null,"abstract":"<div><div>Microplastics (MPs) inevitably undergo aging processes in natural environments; however, how aging behaviors influence the interactions between MPs exposures and nitrate bioreduction in freshwater sediments remains poorly understood. Here, we explored the distinct impacts of virgin and aged MPs (polystyrene (PS) and polylactic acid (PLA)) on nitrate bioreduction processes in lake sediments through a long-term microcosm experiment utilizing the <sup>15</sup>N isotope tracing technique and molecular analysis. Compared to virgin MPs, aged PLA significantly increased the rates of denitrification, anaerobic ammonium oxidation (anammox), and dissimilatory nitrate reduction to ammonium (DNRA) (<em>p</em> &lt; 0.05), facilitating sediment nitrogen loss, while aged PS only significantly improved the rates of DNRA by 272–297 % and contributed to nitrogen retention in sediments. Metagenomic sequencing demonstrated that a more significant enrichment of functional genes responsible for nitrate bioreduction pathways occurred with aged MPs exposures than with virgin MPs. By combining analyses of MPs aging traits and the key drivers of nitrate bioreduction, we revealed that aging behaviors directly regulated sediment nutrient status (e.g., DOC/NO<sub>x</sub><sup>–</sup> ratio) and microbiological properties (from genes to bacteria), thereby further determining the activity of nitrate bioreduction. This work provides new insights into the impacts of aged MPs on sediment nitrate reduction and highlights the role of MPs aging in future assessments of long-term MPs pollution in freshwater ecosystems.</div></div>","PeriodicalId":443,"journal":{"name":"Water Research","volume":"279 ","pages":"Article 123448"},"PeriodicalIF":11.4,"publicationDate":"2025-03-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143560881","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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Water Research
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