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Can Fish Escape the Evolutionary Trap Induced by Microplastics?
IF 9.028 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2025-03-04 DOI: 10.1021/acs.est.4c09932
Weiwenhui Liang, Bowen Li, Amelia Munson, Qiqing Chen, Huahong Shi
Microplastic (MP) ingestion acts as an evolutionary trap with various ecological consequences. Cues that lead animals to respond differently to MPs are key factors driving MP ingestion, yet they remain poorly understood. Here, we quantified the susceptibility of three fish species to different types of MPs across different social contexts. Our results showed that bass were more attracted to MPs that resembled food visually, whereas carp tended to select MPs that shared olfactory cues with food. Goldfish relied more on oral processing to make foraging decisions on MPs. Structural differences in the oropharynx supported these discriminated oral processes. Enlarged group size and fasting time altered the foraging behaviors of MPs of goldfish and bass, both of which were suction-feeding species. Such behavioral changes, regardless of whether fish ultimately ingested or rejected MPs, could pose indirect costs to fish. However, changed group sizes and fasting times did not affect the intake of MPs by the filter-feeding carp. We also proposed four pathways causing the MP-induced evolutionary trap and discussed the potential of fish to escape this trap. Our results contribute to experimental and theoretical understanding of the ecological risks posed by MPs to aquatic species.
{"title":"Can Fish Escape the Evolutionary Trap Induced by Microplastics?","authors":"Weiwenhui Liang, Bowen Li, Amelia Munson, Qiqing Chen, Huahong Shi","doi":"10.1021/acs.est.4c09932","DOIUrl":"https://doi.org/10.1021/acs.est.4c09932","url":null,"abstract":"Microplastic (MP) ingestion acts as an evolutionary trap with various ecological consequences. Cues that lead animals to respond differently to MPs are key factors driving MP ingestion, yet they remain poorly understood. Here, we quantified the susceptibility of three fish species to different types of MPs across different social contexts. Our results showed that bass were more attracted to MPs that resembled food visually, whereas carp tended to select MPs that shared olfactory cues with food. Goldfish relied more on oral processing to make foraging decisions on MPs. Structural differences in the oropharynx supported these discriminated oral processes. Enlarged group size and fasting time altered the foraging behaviors of MPs of goldfish and bass, both of which were suction-feeding species. Such behavioral changes, regardless of whether fish ultimately ingested or rejected MPs, could pose indirect costs to fish. However, changed group sizes and fasting times did not affect the intake of MPs by the filter-feeding carp. We also proposed four pathways causing the MP-induced evolutionary trap and discussed the potential of fish to escape this trap. Our results contribute to experimental and theoretical understanding of the ecological risks posed by MPs to aquatic species.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"33 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-03-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143546061","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
Heating-Induced Changes in Content and Molecular Characteristics of Pyrogenic Dissolved Organic Matter across Soil Types.
IF 10.8 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2025-03-04 Epub Date: 2025-02-19 DOI: 10.1021/acs.est.4c08306
Qiang Zhang, Yinghui Wang, Yuhang Zhang, Junwen Zhang, Fuyou Hou, Chen He, Quan Shi, Gan Zhang, Junjian Wang

Wildfires remarkably alter the quantity and quality of dissolved organic matter (DOM) that regulates postfire biogeochemical processes and environmental quality. However, it remains unclear how the heating-induced percent changes (%HIC) in DOM quantity and quality differ among soil types on a wide geographic scale. Here, we used dissolved organic carbon (DOC) quantification, absorption, and fluorescence spectroscopies, and Fourier transform ion cyclotron resonance mass spectrometry to investigate the variations in %HIC in DOM quantity and quality of Chinese soil reference materials after heating at 250 and 400 °C. Our results reveal that as soil pH increased, %HIC in DOC content increased, while %HIC in aromaticity-related indices of DOM decreased for both heating temperatures. Moreover, the %HIC in DOM biolability and contents of aliphatics increased with soil pH for 250 °C heating but remained relatively stable for 400 °C heating. Results suggest that compared to those in acidic soil-dominated forests, wildfires in alkaline soil-dominated forests may cause greater DOM content and biolability in soils, which may facilitate postfire microbial recovery. These findings deepen our understanding of the site-specific impacts of wildfires on DOM and the subsequent implications for biogeochemical cycling and environmental quality across different geographic regions.

{"title":"Heating-Induced Changes in Content and Molecular Characteristics of Pyrogenic Dissolved Organic Matter across Soil Types.","authors":"Qiang Zhang, Yinghui Wang, Yuhang Zhang, Junwen Zhang, Fuyou Hou, Chen He, Quan Shi, Gan Zhang, Junjian Wang","doi":"10.1021/acs.est.4c08306","DOIUrl":"10.1021/acs.est.4c08306","url":null,"abstract":"<p><p>Wildfires remarkably alter the quantity and quality of dissolved organic matter (DOM) that regulates postfire biogeochemical processes and environmental quality. However, it remains unclear how the heating-induced percent changes (%HIC) in DOM quantity and quality differ among soil types on a wide geographic scale. Here, we used dissolved organic carbon (DOC) quantification, absorption, and fluorescence spectroscopies, and Fourier transform ion cyclotron resonance mass spectrometry to investigate the variations in %HIC in DOM quantity and quality of Chinese soil reference materials after heating at 250 and 400 °C. Our results reveal that as soil pH increased, %HIC in DOC content increased, while %HIC in aromaticity-related indices of DOM decreased for both heating temperatures. Moreover, the %HIC in DOM biolability and contents of aliphatics increased with soil pH for 250 °C heating but remained relatively stable for 400 °C heating. Results suggest that compared to those in acidic soil-dominated forests, wildfires in alkaline soil-dominated forests may cause greater DOM content and biolability in soils, which may facilitate postfire microbial recovery. These findings deepen our understanding of the site-specific impacts of wildfires on DOM and the subsequent implications for biogeochemical cycling and environmental quality across different geographic regions.</p>","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":" ","pages":"3937-3948"},"PeriodicalIF":10.8,"publicationDate":"2025-03-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143447275","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
Mixed Model Approaches Can Leverage Database Information to Improve the Estimation of Size-Adjusted Contaminant Concentrations in Fish Populations
IF 9.028 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2025-03-04 DOI: 10.1021/acs.est.4c10303
Emily Smenderovac, Brian W. Kielstra, Calvin Kluke, Thomas A. Johnston, Satyendra P. Bhavsar, Robert Mackereth, Stephanie Melles, Gretchen L. Lescord, Erik J. S. Emilson
Concentrations of bioaccumulative contaminants in fish increase with their size and age; thus, research and monitoring of these contaminants in fish across space and time can be confounded by size covariation. To account for this, size-standardization of contaminant concentrations within fish samples is a common practice. Standardized concentrations are often estimated using within-sample regression models, also known as power series regression (referred to here as sampling event regressions, or SERs). This approach requires higher sample sizes than mixed effect models (MEMs), which are suited for this application but are not as commonly used. Herein we compare SERs to three MEM approaches; restricted maximum likelihood, Bayesian inference via Markov chain Monte Carlo (MCMC), and approximate Bayesian inference with nested Laplace approximation (INLA). We did this for two contaminants: mercury (Hg), a contaminant known to bioaccumulate, and arsenic (As), where the bioaccumulative potential is less understood. The MEM approaches generated size-standardized concentrations for small populations (e.g., <5 fish) and/or populations that lacked the range of sizes required for SER estimates, with comparable residual and root mean squared error to SER estimates. INLA was determined to be the best method in most cases because it was computationally less intensive than other approaches and showed consistent performance across a range of scenarios with sample-size limitations. Additionally, we provided example code for prediction using the R-INLA package to enable use and application in fisheries’ contaminant monitoring and research.
{"title":"Mixed Model Approaches Can Leverage Database Information to Improve the Estimation of Size-Adjusted Contaminant Concentrations in Fish Populations","authors":"Emily Smenderovac, Brian W. Kielstra, Calvin Kluke, Thomas A. Johnston, Satyendra P. Bhavsar, Robert Mackereth, Stephanie Melles, Gretchen L. Lescord, Erik J. S. Emilson","doi":"10.1021/acs.est.4c10303","DOIUrl":"https://doi.org/10.1021/acs.est.4c10303","url":null,"abstract":"Concentrations of bioaccumulative contaminants in fish increase with their size and age; thus, research and monitoring of these contaminants in fish across space and time can be confounded by size covariation. To account for this, size-standardization of contaminant concentrations within fish samples is a common practice. Standardized concentrations are often estimated using within-sample regression models, also known as power series regression (referred to here as sampling event regressions, or SERs). This approach requires higher sample sizes than mixed effect models (MEMs), which are suited for this application but are not as commonly used. Herein we compare SERs to three MEM approaches; restricted maximum likelihood, Bayesian inference via Markov chain Monte Carlo (MCMC), and approximate Bayesian inference with nested Laplace approximation (INLA). We did this for two contaminants: mercury (Hg), a contaminant known to bioaccumulate, and arsenic (As), where the bioaccumulative potential is less understood. The MEM approaches generated size-standardized concentrations for small populations (e.g., &lt;5 fish) and/or populations that lacked the range of sizes required for SER estimates, with comparable residual and root mean squared error to SER estimates. INLA was determined to be the best method in most cases because it was computationally less intensive than other approaches and showed consistent performance across a range of scenarios with sample-size limitations. Additionally, we provided example code for prediction using the R-INLA package to enable use and application in fisheries’ contaminant monitoring and research.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"423 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-03-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143546077","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
Entropy Similarity-Driven Transformation Reaction Molecular Networking Reveals Transformation Pathways and Potential Risks of Emerging Contaminants in Wastewater: The Example of Sartans.
IF 10.8 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2025-03-04 Epub Date: 2025-02-19 DOI: 10.1021/acs.est.4c13144
Yuli Qian, Yunhao Ke, Liye Wang, Nanyang Yu, Yujie He, Qingmiao Yu, Si Wei, Hongqiang Ren, Jinju Geng

The transformation pathways and risks of emerging contaminants (ECs) in wastewater remain unclear due to the limited throughput of nontarget screening. In this study, an improved method called entropy similarity-driven transformation reaction molecular networking (ESTRMN) was developed to identify transformation products (TPs) in wastewater. In detail, entropy similarity was the most effective algorithm for identifying parent-product spectrum pairs and a threshold of 0.5 for it was determined with the guarantee of high specificity. Additionally, a TP structure database predicted according to known structures and reactions was established to assist in identification. Sartan is one of the most commonly used angiotensin II receptor blocker antihypertensive drugs. Take sartans as an example, 69 TPs of sartans with confidence levels above 3 were identified by ESTRMN, 43 of which were newly discovered. The most common reactions included hydroxylation, hydrolysis, and oxidation, resulting in the majority of sartan TPs exhibiting higher persistence, mobility, and toxicity (PMT) than their parents. The concentration of 75% sartans and TPs increased after treatment in a WWTP, and the overall risk has not been effectively mitigated. This study emphasizes the role of ESTRMN in incorporating TPs of ECs into environmental monitoring protocols and risk assessment frameworks for wastewater management.

{"title":"Entropy Similarity-Driven Transformation Reaction Molecular Networking Reveals Transformation Pathways and Potential Risks of Emerging Contaminants in Wastewater: The Example of Sartans.","authors":"Yuli Qian, Yunhao Ke, Liye Wang, Nanyang Yu, Yujie He, Qingmiao Yu, Si Wei, Hongqiang Ren, Jinju Geng","doi":"10.1021/acs.est.4c13144","DOIUrl":"10.1021/acs.est.4c13144","url":null,"abstract":"<p><p>The transformation pathways and risks of emerging contaminants (ECs) in wastewater remain unclear due to the limited throughput of nontarget screening. In this study, an improved method called entropy similarity-driven transformation reaction molecular networking (ESTRMN) was developed to identify transformation products (TPs) in wastewater. In detail, entropy similarity was the most effective algorithm for identifying parent-product spectrum pairs and a threshold of 0.5 for it was determined with the guarantee of high specificity. Additionally, a TP structure database predicted according to known structures and reactions was established to assist in identification. Sartan is one of the most commonly used angiotensin II receptor blocker antihypertensive drugs. Take sartans as an example, 69 TPs of sartans with confidence levels above 3 were identified by ESTRMN, 43 of which were newly discovered. The most common reactions included hydroxylation, hydrolysis, and oxidation, resulting in the majority of sartan TPs exhibiting higher persistence, mobility, and toxicity (PMT) than their parents. The concentration of 75% sartans and TPs increased after treatment in a WWTP, and the overall risk has not been effectively mitigated. This study emphasizes the role of ESTRMN in incorporating TPs of ECs into environmental monitoring protocols and risk assessment frameworks for wastewater management.</p>","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":" ","pages":"4153-4164"},"PeriodicalIF":10.8,"publicationDate":"2025-03-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143447273","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
Photodegradation of Chlorinated Persistent Organic Pollutants (Cl-POPs) in Pearl River Suspended Particulate Matter-Water Systems: Kinetics, Quantitative Structure-Activity Relationship (QSAR) Development, and Mechanism.
IF 10.8 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2025-03-04 Epub Date: 2025-02-19 DOI: 10.1021/acs.est.4c07246
Xiaolei Teng, Jianqiao Xu, Zunyao Wang, Ruijuan Qu

Chlorinated persistent organic pollutants (Cl-POPs) are highly hydrophobic and are easily adsorbed to solid particulate matter after being released into the water column, thus affecting the transformation process and environmental fate. This study investigated the photodegradation behavior of 16 Cl-POPs in the Pearl River suspended particulate matter (SPM)-water system. The photodegradation rates of polychlorinated biphenyls (PCBs) were generally higher than those of dioxins and increased with substitution numbers of Cl atoms. A QSAR model correlating photodegradation rate constants of Cl-POPs and their structural parameters was established by using multiple linear regression (MLR) analysis and machine learning. The model results showed that soil-water partition coefficient (KOC), morgan fingerprint (mf_1747), and nucleophilicity index (NI) were the main factors affecting the photodegradation of Cl-POPs, confirming that the photodegradation of Cl-POPs with higher hydrophobicity and larger nucleophilic reactivity proceeded faster. According to the quenching experiment and theoretical calculation results, O2- in the hydrophobic region contributed more to the strongly hydrophobic Cl-POPs, while the contribution of OH was mainly concentrated in the weakly hydrophobic Cl-POPs. This study provided valuable insights into photolysis-related environmental persistence and fate of Cl-POPs in the SPM-water system.

{"title":"Photodegradation of Chlorinated Persistent Organic Pollutants (Cl-POPs) in Pearl River Suspended Particulate Matter-Water Systems: Kinetics, Quantitative Structure-Activity Relationship (QSAR) Development, and Mechanism.","authors":"Xiaolei Teng, Jianqiao Xu, Zunyao Wang, Ruijuan Qu","doi":"10.1021/acs.est.4c07246","DOIUrl":"10.1021/acs.est.4c07246","url":null,"abstract":"<p><p>Chlorinated persistent organic pollutants (Cl-POPs) are highly hydrophobic and are easily adsorbed to solid particulate matter after being released into the water column, thus affecting the transformation process and environmental fate. This study investigated the photodegradation behavior of 16 Cl-POPs in the Pearl River suspended particulate matter (SPM)-water system. The photodegradation rates of polychlorinated biphenyls (PCBs) were generally higher than those of dioxins and increased with substitution numbers of Cl atoms. A QSAR model correlating photodegradation rate constants of Cl-POPs and their structural parameters was established by using multiple linear regression (MLR) analysis and machine learning. The model results showed that soil-water partition coefficient (<i>K</i><sub>OC</sub>), morgan fingerprint (mf_1747), and nucleophilicity index (NI) were the main factors affecting the photodegradation of Cl-POPs, confirming that the photodegradation of Cl-POPs with higher hydrophobicity and larger nucleophilic reactivity proceeded faster. According to the quenching experiment and theoretical calculation results, <sup>•</sup>O<sub>2</sub><sup>-</sup> in the hydrophobic region contributed more to the strongly hydrophobic Cl-POPs, while the contribution of <sup>•</sup>OH was mainly concentrated in the weakly hydrophobic Cl-POPs. This study provided valuable insights into photolysis-related environmental persistence and fate of Cl-POPs in the SPM-water system.</p>","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":" ","pages":"4059-4067"},"PeriodicalIF":10.8,"publicationDate":"2025-03-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143447276","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
Characterizing Seasonal Patterns, Gas-Particle Partitioning, and Potential Sources of Airborne Per- and Polyfluoroalkyl Substances in Japan
IF 9.028 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2025-03-04 DOI: 10.1021/acs.est.4c14109
Daichi Asakawa, Huiju Lin, Yuefei Ruan, Sachi Taniyasu, Leo W. Y. Yeung, Toshiki Tojo, Makiko Ichihara, Eriko Yamazaki, Nobuyasu Hanari, Paul K. S. Lam, Nobuyoshi Yamashita
The global ubiquity of perfluoroalkyl and polyfluoroalkyl substances (PFAS) highlights the important role of atmospheric transport. This study monitored 47 PFAS, including perfluoroalkyl acids (PFAAs), emerging PFAS, and precursors of PFAAs (pre-PFAAs), in seasonal ambient air in Japan between 2022 and 2023, quantifying 38 of them in collected samples. The profiles were dominated by 6:2 fluorotelomer alcohol, perfluorobutanesulfonic acid, and perfluorobutanoic acid, with median levels of 245, 117, and 78.0 pg m–3, respectively. Pre-PFAS and perfluoroalkyl carboxylic acids (PFCAs) exhibited relatively higher concentrations in the warm seasons, whereas perfluoroalkyl sulfonic acids (PFSAs) were more abundant in the cold seasons. Particle-bound fractions of PFCAs with carbon number (Cn) ≤ 13 and PFSAs with Cn ≤ 8 were found at lower levels than in previous reports. Additionally, an odd–even pattern in the gas-particle distribution ratio was observed for PFCAs, with relatively higher values for odd-numbered compounds than for their even-numbered counterparts. Using positive matrix factorization analysis, aqueous film-forming foam-related activities, waste stream emissions, and fluoropolymer manufacturing were proposed as potential major sources in the studied areas, with their relative contribution quantified. These findings enhance our understanding of the atmospheric behavior of PFAS and facilitate the development of tailored PFAS mitigation strategies.
{"title":"Characterizing Seasonal Patterns, Gas-Particle Partitioning, and Potential Sources of Airborne Per- and Polyfluoroalkyl Substances in Japan","authors":"Daichi Asakawa, Huiju Lin, Yuefei Ruan, Sachi Taniyasu, Leo W. Y. Yeung, Toshiki Tojo, Makiko Ichihara, Eriko Yamazaki, Nobuyasu Hanari, Paul K. S. Lam, Nobuyoshi Yamashita","doi":"10.1021/acs.est.4c14109","DOIUrl":"https://doi.org/10.1021/acs.est.4c14109","url":null,"abstract":"The global ubiquity of perfluoroalkyl and polyfluoroalkyl substances (PFAS) highlights the important role of atmospheric transport. This study monitored 47 PFAS, including perfluoroalkyl acids (PFAAs), emerging PFAS, and precursors of PFAAs (<i>pre</i>-PFAAs), in seasonal ambient air in Japan between 2022 and 2023, quantifying 38 of them in collected samples. The profiles were dominated by 6:2 fluorotelomer alcohol, perfluorobutanesulfonic acid, and perfluorobutanoic acid, with median levels of 245, 117, and 78.0 pg m<sup>–3</sup>, respectively. <i>Pre-</i>PFAS and perfluoroalkyl carboxylic acids (PFCAs) exhibited relatively higher concentrations in the warm seasons, whereas perfluoroalkyl sulfonic acids (PFSAs) were more abundant in the cold seasons. Particle-bound fractions of PFCAs with carbon number (<i>C</i><sub>n</sub>) ≤ 13 and PFSAs with <i>C</i><sub>n</sub> ≤ 8 were found at lower levels than in previous reports. Additionally, an odd–even pattern in the gas-particle distribution ratio was observed for PFCAs, with relatively higher values for odd-numbered compounds than for their even-numbered counterparts. Using positive matrix factorization analysis, aqueous film-forming foam-related activities, waste stream emissions, and fluoropolymer manufacturing were proposed as potential major sources in the studied areas, with their relative contribution quantified. These findings enhance our understanding of the atmospheric behavior of PFAS and facilitate the development of tailored PFAS mitigation strategies.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"52 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-03-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143546078","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
Biofilm-Induced Critical Flux in Dead-End Ultrafiltration Processes: Phenomenon, Mechanism, and Economic and Environmental Benefits
IF 9.028 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2025-03-03 DOI: 10.1021/acs.est.4c11760
Keying Xiong, Li Long, Juntao Xing, Liang Luo, Chu Zhou, Xu Wang, Senlin Shao
The concept of critical flux, introduced by R.W. Field, defines the flux below which the filtration resistance remains constant over time. Notably, this concept, originally for cross-flow filtration, faces challenges in dead-end filtration (the dominant mode used in drinking water ultrafiltration (UF)). Herein, leveraged by regulated membrane biofilms, we proposed a novel biofilm-induced critical flux specific to dead-end filtration. Below this critical flux, the membrane biofilm could act like a cross-flow to maintain mass balances by the biodegradation of foulants, thereby preventing a continuous increase in filtration resistance. Additionally, we demonstrated an optimized strategy to improve the critical flux─backwashing without air scouring, which doubled the critical flux from 6 to 12 L·m–2·h–1. A life cycle analysis revealed that operating at the biofilm-induced critical flux can reduce energy consumption and minimize membrane cleaning, thereby effectively lowering the overall operating costs (52%) and carbon emissions (61%) compared to conventional UF. Sensitivity analysis also indicated that extending membrane life and reducing membrane costs were crucial for lowering overall operating costs, while minimizing fossil energy usage was decisive for reducing carbon emissions. Overall, our study demonstrates that operating at a biofilm-induced critical flux offers a low-maintenance, cost-effective, and environmentally sustainable strategy for drinking water UF.
{"title":"Biofilm-Induced Critical Flux in Dead-End Ultrafiltration Processes: Phenomenon, Mechanism, and Economic and Environmental Benefits","authors":"Keying Xiong, Li Long, Juntao Xing, Liang Luo, Chu Zhou, Xu Wang, Senlin Shao","doi":"10.1021/acs.est.4c11760","DOIUrl":"https://doi.org/10.1021/acs.est.4c11760","url":null,"abstract":"The concept of critical flux, introduced by R.W. Field, defines the flux below which the filtration resistance remains constant over time. Notably, this concept, originally for cross-flow filtration, faces challenges in dead-end filtration (the dominant mode used in drinking water ultrafiltration (UF)). Herein, leveraged by regulated membrane biofilms, we proposed a novel biofilm-induced critical flux specific to dead-end filtration. Below this critical flux, the membrane biofilm could act like a cross-flow to maintain mass balances by the biodegradation of foulants, thereby preventing a continuous increase in filtration resistance. Additionally, we demonstrated an optimized strategy to improve the critical flux─backwashing without air scouring, which doubled the critical flux from 6 to 12 L·m<sup>–2</sup>·h<sup>–1</sup>. A life cycle analysis revealed that operating at the biofilm-induced critical flux can reduce energy consumption and minimize membrane cleaning, thereby effectively lowering the overall operating costs (52%) and carbon emissions (61%) compared to conventional UF. Sensitivity analysis also indicated that extending membrane life and reducing membrane costs were crucial for lowering overall operating costs, while minimizing fossil energy usage was decisive for reducing carbon emissions. Overall, our study demonstrates that operating at a biofilm-induced critical flux offers a low-maintenance, cost-effective, and environmentally sustainable strategy for drinking water UF.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"34 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-03-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143532716","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
Acute Impact of Nonoptimal Ambient Temperatures on Plasma Levels of 3000 Proteins in Chinese Adults 非最佳环境温度对中国成年人血浆中 3000 种蛋白质水平的急性影响
IF 9.028 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2025-03-03 DOI: 10.1021/acs.est.4c13020
Yi Tong Guo, Mohsen Mazidi, Neil Wright, Pang Yao, Baihan Wang, Yue Niu, Xi Xia, Xia Meng, Cong Liu, Robert Clarke, Kin Bong Hubert Lam, Christiana Kartsonaki, Iona Millwood, Yiping Chen, Ling Yang, Huaidong Du, Canqing Yu, Dianjianyi Sun, Jun Lv, Liming Li, Junshi Chen, Maxim Barnard, Xiaocao Tian, Kin Fai Ho, Ka Hung Chan, Antonio Gasparrini, Haidong Kan, Zhengming Chen, the China Kadoorie Biobank Study Group
Nonoptimal ambient temperatures (i.e., cold and heat) are leading environmental determinants of major diseases worldwide, but the underlying pathological mechanisms are still poorly understood. We used distributed-lag nonlinear models to examine the associations of cold (5th percentile: −2.1 °C) and heat (95th percentile: 29.5 °C) with 2923 plasma proteins in 3926 adults from 10 areas across China. Overall, 949 proteins were significantly (5% false discovery rate) associated with ambient temperature, including 387 (216/171 down/upregulated) with cold, 770 (656/114 down/upregulated) with heat, and 208 with both cold and heat. Above the median reference temperature (17.7 °C), the associations were largely linear, while below it, they were nonlinear with attenuation below 5 °C, potentially reflecting mediation by heating. Among the 949 proteins, >80% were also associated with systolic blood pressure and incident ischemic heart disease risk and enriched in relevant pathological pathways (e.g., inflammation, immunity, and platelet aggregation). Our study provided a novel atlas of plasma proteins associated with nonoptimal temperatures in Chinese adults.
{"title":"Acute Impact of Nonoptimal Ambient Temperatures on Plasma Levels of 3000 Proteins in Chinese Adults","authors":"Yi Tong Guo, Mohsen Mazidi, Neil Wright, Pang Yao, Baihan Wang, Yue Niu, Xi Xia, Xia Meng, Cong Liu, Robert Clarke, Kin Bong Hubert Lam, Christiana Kartsonaki, Iona Millwood, Yiping Chen, Ling Yang, Huaidong Du, Canqing Yu, Dianjianyi Sun, Jun Lv, Liming Li, Junshi Chen, Maxim Barnard, Xiaocao Tian, Kin Fai Ho, Ka Hung Chan, Antonio Gasparrini, Haidong Kan, Zhengming Chen, the China Kadoorie Biobank Study Group","doi":"10.1021/acs.est.4c13020","DOIUrl":"https://doi.org/10.1021/acs.est.4c13020","url":null,"abstract":"Nonoptimal ambient temperatures (i.e., cold and heat) are leading environmental determinants of major diseases worldwide, but the underlying pathological mechanisms are still poorly understood. We used distributed-lag nonlinear models to examine the associations of cold (5<sup>th</sup> percentile: −2.1 °C) and heat (95<sup>th</sup> percentile: 29.5 °C) with 2923 plasma proteins in 3926 adults from 10 areas across China. Overall, 949 proteins were significantly (5% false discovery rate) associated with ambient temperature, including 387 (216/171 down/upregulated) with cold, 770 (656/114 down/upregulated) with heat, and 208 with both cold and heat. Above the median reference temperature (17.7 °C), the associations were largely linear, while below it, they were nonlinear with attenuation below 5 °C, potentially reflecting mediation by heating. Among the 949 proteins, &gt;80% were also associated with systolic blood pressure and incident ischemic heart disease risk and enriched in relevant pathological pathways (e.g., inflammation, immunity, and platelet aggregation). Our study provided a novel atlas of plasma proteins associated with nonoptimal temperatures in Chinese adults.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"67 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-03-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143539242","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
Biodegradation of Hexagonal Boron Nitride Nanomaterials by Neutrophils
IF 9.028 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2025-03-03 DOI: 10.1021/acs.est.4c13298
Zhuomiao Liu, Jian Zhao, Liyun Yin, Kun Wang, Hao Feng, Lingzhi Li, Sicheng Xiong, Xinyue Li, Xia Liu, Yanhui Dai, Tongtao Yue, Zhenyu Wang, Baoshan Xing
The biodegradation of hexagonal boron nitride (h-BN) nanomaterials by neutrophils was investigated. After incubation for 36 h, h-BN nanosheets are taken up by neutrophils, and their structure is highly disrupted, as observed via high-resolution transmission electron microscopy (HR-TEM) and confocal Raman imaging. Among the three degradation pathways, the release of neutrophil extracellular traps from neutrophils is the dominant, with myeloperoxidase (MPO) playing an important role. Molecular dynamics simulations show that MPO spontaneously attach onto h-BN surface, and leverage the active sites of MPO to form favorable contacts with h-BN to initiate the degradation. Hypochlorite produced by MPO is responsible for h-BN degradation. With the assistance of hypochlorite, B–O and N–O bonds are formed on h-BN, along with B–N bond breakage and the release of ionic boron and nitrogen based on byproduct identification and first-principle calculations. Additionally, h-BN nanosheets are significantly degraded into small pieces, and the particle concentration of h-BN with a size of 0–100 nm increases by 58.7% after degradation. Following degradation, h-BN nanosheets induce significant hemolysis of red blood cells, and exhibit higher cytotoxicity against epithelial cells. Our findings highlight the importance of considering h-BN degradation for its safe application, and demonstrate the actual risk of h-BN in biological and natural environments.
{"title":"Biodegradation of Hexagonal Boron Nitride Nanomaterials by Neutrophils","authors":"Zhuomiao Liu, Jian Zhao, Liyun Yin, Kun Wang, Hao Feng, Lingzhi Li, Sicheng Xiong, Xinyue Li, Xia Liu, Yanhui Dai, Tongtao Yue, Zhenyu Wang, Baoshan Xing","doi":"10.1021/acs.est.4c13298","DOIUrl":"https://doi.org/10.1021/acs.est.4c13298","url":null,"abstract":"The biodegradation of hexagonal boron nitride (h-BN) nanomaterials by neutrophils was investigated. After incubation for 36 h, h-BN nanosheets are taken up by neutrophils, and their structure is highly disrupted, as observed via high-resolution transmission electron microscopy (HR-TEM) and confocal Raman imaging. Among the three degradation pathways, the release of neutrophil extracellular traps from neutrophils is the dominant, with myeloperoxidase (MPO) playing an important role. Molecular dynamics simulations show that MPO spontaneously attach onto h-BN surface, and leverage the active sites of MPO to form favorable contacts with h-BN to initiate the degradation. Hypochlorite produced by MPO is responsible for h-BN degradation. With the assistance of hypochlorite, B–O and N–O bonds are formed on h-BN, along with B–N bond breakage and the release of ionic boron and nitrogen based on byproduct identification and first-principle calculations. Additionally, h-BN nanosheets are significantly degraded into small pieces, and the particle concentration of h-BN with a size of 0–100 nm increases by 58.7% after degradation. Following degradation, h-BN nanosheets induce significant hemolysis of red blood cells, and exhibit higher cytotoxicity against epithelial cells. Our findings highlight the importance of considering h-BN degradation for its safe application, and demonstrate the actual risk of h-BN in biological and natural environments.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"1 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-03-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143532714","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
Hydrated Electrons Trigger the Breakdown of Recalcitrant Cyanuric Acid in Wastewater
IF 9.028 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2025-03-03 DOI: 10.1021/acs.est.4c11652
Xin Luo, Wenxiao Zheng, Qiaoxin Li, Huanxin Ma, Rundong Chen, Xueming Liu, Chunhua Feng
Cyanuric acid (CA), a triazine-ring compound commonly used as a stabilizer for free chlorine to enhance disinfection, often persists in wastewater for the production of chlorinated cyanurates (Cl-CAs), posing challenges for treatment. This study demonstrates that conventional advanced oxidation processes (UV/H2O2 and UV/peroxydisulfate) are ineffective in degrading CA, while the UV/sulfite system successfully achieves its breakdown. Hydrated electrons (eaq) were identified as the primary reactive species responsible for cleaving the stable triazine ring, with minimal contributions from SO3•– and H. The pH value influences both the activity of eaq and the degradability of CA by altering its structure; lower pH increases the electron-deficient regions in dihydrogen CA, enhancing its susceptibility to nucleophilic attack by eaq. The high concentrations of Cl can inhibit CA removal, likely due to the formation of reactive chlorine species that react with sulfite and suppress eaq production. Effective CA degradation was also demonstrated in real wastewater, highlighting the UV/sulfite system as a sustainable solution for water treatment. These findings offer valuable insights into CA transformation and present effective approaches for eliminating emerging contaminants in the context of the extensive use of disinfectants.
{"title":"Hydrated Electrons Trigger the Breakdown of Recalcitrant Cyanuric Acid in Wastewater","authors":"Xin Luo, Wenxiao Zheng, Qiaoxin Li, Huanxin Ma, Rundong Chen, Xueming Liu, Chunhua Feng","doi":"10.1021/acs.est.4c11652","DOIUrl":"https://doi.org/10.1021/acs.est.4c11652","url":null,"abstract":"Cyanuric acid (CA), a triazine-ring compound commonly used as a stabilizer for free chlorine to enhance disinfection, often persists in wastewater for the production of chlorinated cyanurates (Cl-CAs), posing challenges for treatment. This study demonstrates that conventional advanced oxidation processes (UV/H<sub>2</sub>O<sub>2</sub> and UV/peroxydisulfate) are ineffective in degrading CA, while the UV/sulfite system successfully achieves its breakdown. Hydrated electrons (e<sub>aq</sub><sup>–</sup>) were identified as the primary reactive species responsible for cleaving the stable triazine ring, with minimal contributions from SO<sub>3</sub><sup>•–</sup> and H<sup>•</sup>. The pH value influences both the activity of e<sub>aq</sub><sup>–</sup> and the degradability of CA by altering its structure; lower pH increases the electron-deficient regions in dihydrogen CA, enhancing its susceptibility to nucleophilic attack by e<sub>aq</sub><sup>–</sup>. The high concentrations of Cl<sup>–</sup> can inhibit CA removal, likely due to the formation of reactive chlorine species that react with sulfite and suppress e<sub>aq</sub><sup>–</sup> production. Effective CA degradation was also demonstrated in real wastewater, highlighting the UV/sulfite system as a sustainable solution for water treatment. These findings offer valuable insights into CA transformation and present effective approaches for eliminating emerging contaminants in the context of the extensive use of disinfectants.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"90 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-03-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143539241","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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