Runa Antony, Pamela E. Rossel, Helen K. Feord, Thorsten Dittmar, Martyn Tranter, Alexandre Magno Anesio, Liane G. Benning
Pigmented microalgae thrive on supraglacial surfaces, producing “sticky” extracellular polymeric substances that combine into a mineral–organic matrix. Together, they enhance snow and ice melting by lowering the albedo. Understanding the chemical nature of particulate organic matter (POM) in this matrix is crucial in assessing its role in supraglacial carbon dynamics. We evaluated POM complexity in alga-rich snow and ice samples containing 0.3–6.4 wt % organic carbon (OC) via extractions with solvents of varying polarity, pH, and OM selectivity. Extraction yields were evaluated by OC analysis of the extracts, and the composition of extracted OM was analyzed using ultrahigh-resolution mass spectrometry. Individual hot water (HW), hydrochloric acid (HCl), and sodium hydroxide (NaOH) extractions achieved up to 87% efficiency, outperforming sequential, organic solvent-based extractions (<11%). OM extracted by HW, HCl, and NaOH combined had more molecular formulas (2827) than OM extracted with organic solvents (1926 formulas). Combined HW, NaOH, and HCl extractions yielded an OM composition with unsaturated, highly unsaturated, aromatic, and N-containing compounds, while unsaturated aliphatics and black carbon-derived polycyclic aromatics were enriched in the organic solvent extracts. This molecular profiling provides the first comprehensive insights into supraglacial POM composition, opening the window for understanding its role in the cryospheric carbon cycle.
{"title":"Extraction Strategies for Profiling the Molecular Composition of Particulate Organic Matter on Glacier Surfaces","authors":"Runa Antony, Pamela E. Rossel, Helen K. Feord, Thorsten Dittmar, Martyn Tranter, Alexandre Magno Anesio, Liane G. Benning","doi":"10.1021/acs.est.4c10088","DOIUrl":"https://doi.org/10.1021/acs.est.4c10088","url":null,"abstract":"Pigmented microalgae thrive on supraglacial surfaces, producing “sticky” extracellular polymeric substances that combine into a mineral–organic matrix. Together, they enhance snow and ice melting by lowering the albedo. Understanding the chemical nature of particulate organic matter (POM) in this matrix is crucial in assessing its role in supraglacial carbon dynamics. We evaluated POM complexity in alga-rich snow and ice samples containing 0.3–6.4 wt % organic carbon (OC) via extractions with solvents of varying polarity, pH, and OM selectivity. Extraction yields were evaluated by OC analysis of the extracts, and the composition of extracted OM was analyzed using ultrahigh-resolution mass spectrometry. Individual hot water (HW), hydrochloric acid (HCl), and sodium hydroxide (NaOH) extractions achieved up to 87% efficiency, outperforming sequential, organic solvent-based extractions (<11%). OM extracted by HW, HCl, and NaOH combined had more molecular formulas (2827) than OM extracted with organic solvents (1926 formulas). Combined HW, NaOH, and HCl extractions yielded an OM composition with unsaturated, highly unsaturated, aromatic, and N-containing compounds, while unsaturated aliphatics and black carbon-derived polycyclic aromatics were enriched in the organic solvent extracts. This molecular profiling provides the first comprehensive insights into supraglacial POM composition, opening the window for understanding its role in the cryospheric carbon cycle.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"141 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-02-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143518120","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}
Ayoub Moradi, Temesgen Alemayehu Abera, Elliot Samuel Shayle, Mohammed Ahmed Muhammed, Dirk Zeuss
Biogenic Volatile Organic Compounds (BVOCs) are organic chemicals emitted primarily by flora. They impact climate and human health, and their presence is influenced by environmental conditions. Despite the intense effects of climate change, there is lack of information about the spatiotemporal variations in BVOC emissions and underlying driving factors. This study aims to quantify the variation of BVOCs in Germany and attribute it to deriving factors. We first conducted a detailed study covering the period from 1979 to 2024, during which satellite observations were first became available. Then, using historical records and projected future climate-change scenarios, we simulated the dynamics of BVOCs over an extended timeframe (1790–2065). To track changes in BVOCs emissions, we accounted for constant emission factors and used remotely sensed proxies, summarized into five main factors: biomass, temperature, carbon dioxide, soil moisture, and wildfire. Our results show that the trend of BVOCs emissions declining reversed in 1978 ± 1, with increases now being observed. Since this year, the average BVOCs emissions in Germany increased by ∼54%. Spatially, eastern-central Germany and urban areas exhibit the highest increase. Future projections indicate a continued increase in emissions over the coming decades. Our results were validated by analyzing the Total Column Ozone and Formaldehyde.
{"title":"Modeling Long-Term Dynamics of Biogenic Volatile Organic Compounds (BVOCs) in Germany Based on Major Precursors","authors":"Ayoub Moradi, Temesgen Alemayehu Abera, Elliot Samuel Shayle, Mohammed Ahmed Muhammed, Dirk Zeuss","doi":"10.1021/acs.est.4c14418","DOIUrl":"https://doi.org/10.1021/acs.est.4c14418","url":null,"abstract":"Biogenic Volatile Organic Compounds (BVOCs) are organic chemicals emitted primarily by flora. They impact climate and human health, and their presence is influenced by environmental conditions. Despite the intense effects of climate change, there is lack of information about the spatiotemporal variations in BVOC emissions and underlying driving factors. This study aims to quantify the variation of BVOCs in Germany and attribute it to deriving factors. We first conducted a detailed study covering the period from 1979 to 2024, during which satellite observations were first became available. Then, using historical records and projected future climate-change scenarios, we simulated the dynamics of BVOCs over an extended timeframe (1790–2065). To track changes in BVOCs emissions, we accounted for constant emission factors and used remotely sensed proxies, summarized into five main factors: biomass, temperature, carbon dioxide, soil moisture, and wildfire. Our results show that the trend of BVOCs emissions declining reversed in 1978 ± 1, with increases now being observed. Since this year, the average BVOCs emissions in Germany increased by ∼54%. Spatially, eastern-central Germany and urban areas exhibit the highest increase. Future projections indicate a continued increase in emissions over the coming decades. Our results were validated by analyzing the Total Column Ozone and Formaldehyde.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"27 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-02-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143495393","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}
Susan Richardson, Xingfang Li, William Mitch, Xiangru Zhang, Xin Yang, Baiyang Chen, Yang Pan, Wei Wang, Mengting Yang, Huiyu Dong, Jiafu Li
Published as part of <i>Environmental Science & Technology</i> special issue “Celebrating the 50th Anniversary of the Discovery of Drinking Water Disinfection Byproducts”. The year 2024 marked the 50th anniversary of the discovery of disinfection byproducts (DBPs) during drinking water disinfection procedures. The disinfection of drinking water is important for controlling waterborne disease and was used for several decades before DBPs were first discovered in 1974. Initially, chloroform and other trihalomethanes (THMs) were both discovered independently by Rook in The Netherlands (1) and Beller et al. (2) in the United States. Two years later, the U.S. Environmental Protection Agency (EPA) published a national survey showing that chloroform and other THMs were ubiquitous in chlorinated drinking water, (3) and the National Cancer Institute reported that chloroform was carcinogenic in laboratory animals. (4) As a result, an important public health issue was realized, and in 1979, the U.S. EPA issued the first DBP regulation on four THMs in drinking water. Now, most developed countries regulate DBPs, and the World Health Organization has guidelines on maximum allowable exposure levels. However, the reality is that only a tiny fraction of the >700 DBPs now reported (and thousands predicted) are controlled, and many unregulated DBPs are much more toxic than those that are regulated. Moreover, it is still not clear which DBPs are responsible for the bladder cancer, miscarriage, and birth defects reported in human epidemiological studies. Thus, it is clear that there is much work still to do. Environmental Science & Technology (<i>ES&T</i>) and Environmental Science & Technology Letters (<i>ES</i><i>&T Letters</i>) have served a multidisciplinary and diverse audience of chemists, engineers, policymakers, and the broader environmental community over the past decade. Aiming to be both transformational and direction-setting, the two high-impact journals cover a wide range of areas crucial to preserving and restoring human health and the environment. Both journals have joined together to mark this important milestone in disinfection byproduct research, collaborating on an open call for papers for a new special issue entitled “Celebrating the 50th Anniversary of the Discovery of Drinking Water Disinfection Byproducts”. This call for papers invites the latest cutting-edge research and developments shaping this interdisciplinary field. For background context on the most recent advances in this multidisciplinary field over the past five years, the special issue guest editor team has also curated a retrospective collection of <i>ES&T</i> and <i>ES&T Letters</i> papers published between 2020 and 2024 across both journals on this topic. The papers selected showcase the broad and multidisciplinary nature of this field of research, including papers on sources and mechanisms of DBP formation and the relative toxicity of different class
{"title":"Celebrating the 50th Anniversary of the Discovery of Drinking Water Disinfection Byproducts","authors":"Susan Richardson, Xingfang Li, William Mitch, Xiangru Zhang, Xin Yang, Baiyang Chen, Yang Pan, Wei Wang, Mengting Yang, Huiyu Dong, Jiafu Li","doi":"10.1021/acs.est.5c02003","DOIUrl":"https://doi.org/10.1021/acs.est.5c02003","url":null,"abstract":"Published as part of <i>Environmental Science & Technology</i> special issue “Celebrating the 50th Anniversary of the Discovery of Drinking Water Disinfection Byproducts”. The year 2024 marked the 50th anniversary of the discovery of disinfection byproducts (DBPs) during drinking water disinfection procedures. The disinfection of drinking water is important for controlling waterborne disease and was used for several decades before DBPs were first discovered in 1974. Initially, chloroform and other trihalomethanes (THMs) were both discovered independently by Rook in The Netherlands (1) and Beller et al. (2) in the United States. Two years later, the U.S. Environmental Protection Agency (EPA) published a national survey showing that chloroform and other THMs were ubiquitous in chlorinated drinking water, (3) and the National Cancer Institute reported that chloroform was carcinogenic in laboratory animals. (4) As a result, an important public health issue was realized, and in 1979, the U.S. EPA issued the first DBP regulation on four THMs in drinking water. Now, most developed countries regulate DBPs, and the World Health Organization has guidelines on maximum allowable exposure levels. However, the reality is that only a tiny fraction of the >700 DBPs now reported (and thousands predicted) are controlled, and many unregulated DBPs are much more toxic than those that are regulated. Moreover, it is still not clear which DBPs are responsible for the bladder cancer, miscarriage, and birth defects reported in human epidemiological studies. Thus, it is clear that there is much work still to do. Environmental Science & Technology (<i>ES&T</i>) and Environmental Science & Technology Letters (<i>ES</i><i>&T Letters</i>) have served a multidisciplinary and diverse audience of chemists, engineers, policymakers, and the broader environmental community over the past decade. Aiming to be both transformational and direction-setting, the two high-impact journals cover a wide range of areas crucial to preserving and restoring human health and the environment. Both journals have joined together to mark this important milestone in disinfection byproduct research, collaborating on an open call for papers for a new special issue entitled “Celebrating the 50th Anniversary of the Discovery of Drinking Water Disinfection Byproducts”. This call for papers invites the latest cutting-edge research and developments shaping this interdisciplinary field. For background context on the most recent advances in this multidisciplinary field over the past five years, the special issue guest editor team has also curated a retrospective collection of <i>ES&T</i> and <i>ES&T Letters</i> papers published between 2020 and 2024 across both journals on this topic. The papers selected showcase the broad and multidisciplinary nature of this field of research, including papers on sources and mechanisms of DBP formation and the relative toxicity of different class","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"83 1 Pt 2 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-02-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143495394","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}
Rainwater is the primary water source with which terrestrial plastic pollutants interact. Not only could active substances in rainwater generate additional reactive oxygen species but water could also react with the photoaging intermediates of plastic. Precipitation and evaporation lead to repeated shifts between the solid–liquid and solid–gas interfaces during photoaging. To investigate the impact of these interfaces on photoaging, polyvinyl chloride, polypropylene, polystyrene, and polyethylene microplastics were exposed to UVA, UVB, or UVC radiation in common rainwater (CR), rainwater residue (RR), or rainwater-free (RF) treatments. Seasonal field exposure to the corresponding commercial plastics was also conducted. FT-IR spectroscopy was utilized to analyze the chemical changes in both microplastics and commercial plastics. Compared with RF and RR, CR exposure advanced the relative time of carbonyl production in the photoaging process. A model based on local precipitation and radiation data successfully predicted the carbonyl index of field-exposed commercial plastics and highlighted the importance of alternating interface transitions. The increase in the carbonyl index due to each wet–dry cycle was 1.013–5.460 times greater than that of plastics not exposed to rainwater. These findings indicate that plastics undergo different photochemical reactions on different interfaces, and alternating interface transitions can accelerate the photoaging of plastic.
{"title":"Photoaging of Terrestrial Plastic Pollution: A Process Affected by Precipitation","authors":"Jiehan Duan, Danqing Zheng, Yanlin Wu, Mohamad Sleiman, Wenbo Dong","doi":"10.1021/acs.est.4c10844","DOIUrl":"https://doi.org/10.1021/acs.est.4c10844","url":null,"abstract":"Rainwater is the primary water source with which terrestrial plastic pollutants interact. Not only could active substances in rainwater generate additional reactive oxygen species but water could also react with the photoaging intermediates of plastic. Precipitation and evaporation lead to repeated shifts between the solid–liquid and solid–gas interfaces during photoaging. To investigate the impact of these interfaces on photoaging, polyvinyl chloride, polypropylene, polystyrene, and polyethylene microplastics were exposed to UVA, UVB, or UVC radiation in common rainwater (CR), rainwater residue (RR), or rainwater-free (RF) treatments. Seasonal field exposure to the corresponding commercial plastics was also conducted. FT-IR spectroscopy was utilized to analyze the chemical changes in both microplastics and commercial plastics. Compared with RF and RR, CR exposure advanced the relative time of carbonyl production in the photoaging process. A model based on local precipitation and radiation data successfully predicted the carbonyl index of field-exposed commercial plastics and highlighted the importance of alternating interface transitions. The increase in the carbonyl index due to each wet–dry cycle was 1.013–5.460 times greater than that of plastics not exposed to rainwater. These findings indicate that plastics undergo different photochemical reactions on different interfaces, and alternating interface transitions can accelerate the photoaging of plastic.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"53 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-02-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143507299","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}
Léo Chevrier, Sylvain Grangeon, Anthony Beauvois, Eric Bourhis, Jan Filip, Christophe Tournassat
Fe-bearing clay minerals contain structural iron that can be redox-active and can participate in electron transfer reactions with aqueous species. Although these redox properties have been studied extensively in the past decade, questions remain about the respective roles of kinetic and thermodynamic constraints in establishing steady-state redox conditions. In this study, the reduction kinetics of aqueous Cr(VI) to Cr(III) by Fe(II) contained in the structure of reduced ferruginous clay samples (reference Nontronite NAu-1) was monitored with quick-XAS (X-ray absorption spectroscopy). These measurements revealed the occurrence of at least two reaction processes with contrasting fast and slow kinetic rates. According to mass and electron balance calculations, Fe(II) located at the edge of the clay mineral particles alone cannot account for the fast reactivity of the samples, pointing out the presence of electron transfer from the inner part of the clay mineral layer structure to the reactive sites. The Fe(II)/Fe(III) ratio in the clay structure quickly reached a steady state after each Cr(VI) addition to the solution. These steady-state conditions were consistent with either a complete depletion of the Cr(VI) reactant for the first spikes of Cr(VI) or a thermodynamic equilibrium between the redox couples, i.e., between structural Fe(III)/Fe(II) and aqueous Cr(VI)/Cr(III), after the pool of fast-reacting Fe(II) was depleted. These results highlight the need to consider kinetic and thermodynamic controls of clay structural iron redox reactivity to predict the fate of redox-sensitive contaminants in the environment.
{"title":"Probing the Redox Reactivity of a Reduced Nontronite: A Quick XAS Operando Study","authors":"Léo Chevrier, Sylvain Grangeon, Anthony Beauvois, Eric Bourhis, Jan Filip, Christophe Tournassat","doi":"10.1021/acs.est.4c10829","DOIUrl":"https://doi.org/10.1021/acs.est.4c10829","url":null,"abstract":"Fe-bearing clay minerals contain structural iron that can be redox-active and can participate in electron transfer reactions with aqueous species. Although these redox properties have been studied extensively in the past decade, questions remain about the respective roles of kinetic and thermodynamic constraints in establishing steady-state redox conditions. In this study, the reduction kinetics of aqueous Cr(VI) to Cr(III) by Fe(II) contained in the structure of reduced ferruginous clay samples (reference Nontronite NAu-1) was monitored with quick-XAS (X-ray absorption spectroscopy). These measurements revealed the occurrence of at least two reaction processes with contrasting fast and slow kinetic rates. According to mass and electron balance calculations, Fe(II) located at the edge of the clay mineral particles alone cannot account for the fast reactivity of the samples, pointing out the presence of electron transfer from the inner part of the clay mineral layer structure to the reactive sites. The Fe(II)/Fe(III) ratio in the clay structure quickly reached a steady state after each Cr(VI) addition to the solution. These steady-state conditions were consistent with either a complete depletion of the Cr(VI) reactant for the first spikes of Cr(VI) or a thermodynamic equilibrium between the redox couples, i.e., between structural Fe(III)/Fe(II) and aqueous Cr(VI)/Cr(III), after the pool of fast-reacting Fe(II) was depleted. These results highlight the need to consider kinetic and thermodynamic controls of clay structural iron redox reactivity to predict the fate of redox-sensitive contaminants in the environment.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"82 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-02-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143507298","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}
Ashley Heida, Mark T. Hamilton, Julia Gambino, Kaylee Sanderson, Mary E. Schoen, Michael A. Jahne, Jay Garland, Lucia Ramirez, Hunter Quon, Allison J. Lopatkin, Kerry A. Hamilton
Understanding and predicting the role of waterborne environments in transmitting antimicrobial-resistant (AMR) infections are critical for public health. A population ecology-quantitative microbial risk assessment (QMRA) model is proposed to evaluate urinary tract infection (UTI) development due to recreational waterborne exposures to Escherichia coli (E. coli) and antibiotic-resistant extended-spectrum β-lactamase-producing (ESBL) E. coli. The horizontal gene transfer (HGT) mechanism of conjugation and other evolutionary factors were modeled separately in the environment and the gut. Persistence/dilution dominated HGT in the environment; however, HGT highly impacted predicted ESBL populations in the body. Predicted disability life year (DALY) risks from exposure to ESBL E. coli at concentrations consistent with US recreational water criteria were less than the 10–6 pppy benchmark value but greater than the susceptible E. coli DALY risks associated with a UTI health outcome. However, the prevailing susceptible dose–response relationship may underestimate ESBL risk if HGT rates in vivo approach those reported in vitro. A sensitivity analysis demonstrated that DALY values, E. coli/ESBL concentrations, and exposure parameters were influential on predicted risks. The model is a preliminary tool to begin the expansion of the QMRA paradigm to explore the impacts of evolutionary changes in AMR risk assessment.
{"title":"Population Ecology-Quantitative Microbial Risk Assessment (QMRA) Model for Antibiotic-Resistant and Susceptible E. coli in Recreational Water","authors":"Ashley Heida, Mark T. Hamilton, Julia Gambino, Kaylee Sanderson, Mary E. Schoen, Michael A. Jahne, Jay Garland, Lucia Ramirez, Hunter Quon, Allison J. Lopatkin, Kerry A. Hamilton","doi":"10.1021/acs.est.4c07248","DOIUrl":"https://doi.org/10.1021/acs.est.4c07248","url":null,"abstract":"Understanding and predicting the role of waterborne environments in transmitting antimicrobial-resistant (AMR) infections are critical for public health. A population ecology-quantitative microbial risk assessment (QMRA) model is proposed to evaluate urinary tract infection (UTI) development due to recreational waterborne exposures to <i>Escherichia coli</i> (<i>E. coli</i>) and antibiotic-resistant extended-spectrum β-lactamase-producing (ESBL) <i>E. coli</i>. The horizontal gene transfer (HGT) mechanism of conjugation and other evolutionary factors were modeled separately in the environment and the gut. Persistence/dilution dominated HGT in the environment; however, HGT highly impacted predicted ESBL populations in the body. Predicted disability life year (DALY) risks from exposure to ESBL <i>E. coli</i> at concentrations consistent with US recreational water criteria were less than the 10<sup>–6</sup> pppy benchmark value but greater than the susceptible <i>E. coli</i> DALY risks associated with a UTI health outcome. However, the prevailing susceptible dose–response relationship may underestimate ESBL risk if HGT rates <i>in vivo</i> approach those reported <i>in vitro</i>. A sensitivity analysis demonstrated that DALY values, <i>E. coli</i>/ESBL concentrations, and exposure parameters were influential on predicted risks. The model is a preliminary tool to begin the expansion of the QMRA paradigm to explore the impacts of evolutionary changes in AMR risk assessment.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"51 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-02-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143495492","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}
Rational interfacial engineering design of an electrocatalyst, such as a heterojunction structure, can effectively enhance its catalytic activity. This study aims to address a critical challenge associated with the use of carbon material@Ti4O7 heterojunction composite electrodes for wastewater treatment─electrode stability over long-term operation. Herein, we report a highly stabilized interfacial engineering strategy, i.e., the use of conductive inorganic CeO2 as a “cement” to firmly encapsulate N-doped graphene oxide nanosheets (N-GS) on the Ti4O7 surface. The defect-rich N-GS encapsulated on the Ti4O7 surface significantly enhances interfacial charge transfer. This enhancement results in the N-GS/CeO2@Ti4O7 heterojunction composite electrode exhibiting excellent efficiency in the electro-oxidation of hexafluoropropylene oxide dimer acid (HFPO-DA or GenX). Furthermore, a flow-through N-GS/CeO2@Ti4O7 reactive electrochemical membrane system effectively mineralizes other 35 PFASs in a real fluorochemical wastewater sample, achieving a high defluorination rate of 70–90% and exhibiting better performance in PFAS destruction and energy efficiency compared to the UV/KI-SO32– process. Results of this study enhance our understanding of the electrochemical oxidation of PFAS and offer valuable insight into the design of stabilized Ti4O7 heterojunction composites. These findings are instrumental in advancing the development of effective treatments for PFAS-contaminated environments.
{"title":"Durable Ti4O7 Heterojunction Composite Membrane Encapsulating N-Doped Graphene Nanosheets for Efficient Electro-Oxidation of GenX and Other PFAS in Fluorochemical Wastewater","authors":"Yiyang Liang, Anqi Wang, Shangtao Liang, Kai Sun, Ruzhen Xie, Chuanen Zheng, Sihan Zhang, Caiming Tang, Dengmiao Cheng, Jinxia Wang, Qingguo Huang, Hui Lin","doi":"10.1021/acs.est.4c09423","DOIUrl":"https://doi.org/10.1021/acs.est.4c09423","url":null,"abstract":"Rational interfacial engineering design of an electrocatalyst, such as a heterojunction structure, can effectively enhance its catalytic activity. This study aims to address a critical challenge associated with the use of carbon material@Ti<sub>4</sub>O<sub>7</sub> heterojunction composite electrodes for wastewater treatment─electrode stability over long-term operation. Herein, we report a highly stabilized interfacial engineering strategy, i.e., the use of conductive inorganic CeO<sub>2</sub> as a “cement” to firmly encapsulate N-doped graphene oxide nanosheets (N-GS) on the Ti<sub>4</sub>O<sub>7</sub> surface. The defect-rich N-GS encapsulated on the Ti<sub>4</sub>O<sub>7</sub> surface significantly enhances interfacial charge transfer. This enhancement results in the N-GS/CeO<sub>2</sub>@Ti<sub>4</sub>O<sub>7</sub> heterojunction composite electrode exhibiting excellent efficiency in the electro-oxidation of hexafluoropropylene oxide dimer acid (HFPO-DA or GenX). Furthermore, a flow-through N-GS/CeO<sub>2</sub>@Ti<sub>4</sub>O<sub>7</sub> reactive electrochemical membrane system effectively mineralizes other 35 PFASs in a real fluorochemical wastewater sample, achieving a high defluorination rate of 70–90% and exhibiting better performance in PFAS destruction and energy efficiency compared to the UV/KI-SO<sub>3</sub><sup>2–</sup> process. Results of this study enhance our understanding of the electrochemical oxidation of PFAS and offer valuable insight into the design of stabilized Ti<sub>4</sub>O<sub>7</sub> heterojunction composites. These findings are instrumental in advancing the development of effective treatments for PFAS-contaminated environments.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"128 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-02-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143495630","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}
Kentaro Miyazono, Kazuaki Tadokoro, Gajahin G. N. Thushari, Hiroomi Miyamoto, Akinori Takasuka, Mikio Watai, Tohya Yasuda, Takuya Sato, Rei Yamashita, Taketoshi Kodama, Kazutaka Takahashi
Understanding the spatiotemporal dynamics of microplastics on the ocean surface is crucial for assessing their impact on marine ecosystems and human health; however, long-term fluctuations have not been extensively studied. We present a long-term empirical data set on floating marine plastic debris collected from 1949 to 2020 around Japan in the western North Pacific. We observed three phases: 1) a period of increase (0–104 pieces/km2) from the early 1950s to the late 1970s; 2) a stagnation period, with high abundance (104–105 pieces/km2), from the 1980s to the early 2010s; and 3) a period of reincrease (>105 pieces/km2) from the mid-2010s to the present. The shift from film to fragmented plastic in the 1980s and the continuous downsizing may have caused the expansion of the offshore polluted area, resulting in a stagnation period by enhancing removal. The removal is most likely caused by sedimentation with phytoplankton, as the abundance of the plastic debris during this period was significantly related to the winter Pacific Decadal Oscillation, an index of annual primary productivity. The recent increase in microplastics suggests that plastic discharge is outpacing its removal capacity, suggesting that the impact of pollution on ocean surface biota is becoming increasingly evident.
{"title":"Long-Term Changes in the Abundance, Size, and Morphotype of Marine Plastics in the North Pacific","authors":"Kentaro Miyazono, Kazuaki Tadokoro, Gajahin G. N. Thushari, Hiroomi Miyamoto, Akinori Takasuka, Mikio Watai, Tohya Yasuda, Takuya Sato, Rei Yamashita, Taketoshi Kodama, Kazutaka Takahashi","doi":"10.1021/acs.est.4c09706","DOIUrl":"https://doi.org/10.1021/acs.est.4c09706","url":null,"abstract":"Understanding the spatiotemporal dynamics of microplastics on the ocean surface is crucial for assessing their impact on marine ecosystems and human health; however, long-term fluctuations have not been extensively studied. We present a long-term empirical data set on floating marine plastic debris collected from 1949 to 2020 around Japan in the western North Pacific. We observed three phases: 1) a period of increase (0–10<sup>4</sup> pieces/km<sup>2</sup>) from the early 1950s to the late 1970s; 2) a stagnation period, with high abundance (10<sup>4</sup>–10<sup>5</sup> pieces/km<sup>2</sup>), from the 1980s to the early 2010s; and 3) a period of reincrease (>10<sup>5</sup> pieces/km<sup>2</sup>) from the mid-2010s to the present. The shift from film to fragmented plastic in the 1980s and the continuous downsizing may have caused the expansion of the offshore polluted area, resulting in a stagnation period by enhancing removal. The removal is most likely caused by sedimentation with phytoplankton, as the abundance of the plastic debris during this period was significantly related to the winter Pacific Decadal Oscillation, an index of annual primary productivity. The recent increase in microplastics suggests that plastic discharge is outpacing its removal capacity, suggesting that the impact of pollution on ocean surface biota is becoming increasingly evident.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"67 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-02-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143507251","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}
Nicholas Chartres, Max T. Aung, Susan L. Norris, Courtney Cooper, Lisa A. Bero, Roger Chou, Devon C. Payne-Sturges, Wendy E. Wagner, Jessica W. Reyes, Lisa M. Askie, Daniel A. Axelrad, Deysi Flores Vigo, Jill E. Johnston, Juleen Lam, Keeve E. Nachman, Eva Rehfuess, Rachel Rothschild, Patrice Sutton, Lauren Zeise, Tracey J. Woodruff
Environmental exposures, including widespread industrial pollution, impact human health and are amplified in more highly exposed communities. Policy and regulatory frameworks for making decisions and recommendations on interventions to mitigate or prevent exposures tend to narrowly focus on exposure and some health-related data related to risks. Typically, such frameworks do not consider other factors, including essentiality, health equity, and distribution of benefits and costs. Further, decisions and recommendations lack transparency regarding how they were developed. We developed the Navigation Guide Evidence-to-Decision Framework for Environmental Health (E2DFEH) to provide a structured and transparent framework incorporating a range of scientific information and factors for decision-making. We reviewed current evidence-to-decision frameworks and engaged in an iterative consensus-based process involving 30 experts from 25 organizations in the academic, government, and nonprofit sectors. The E2DFEH framework includes three Foundations that are structural factors considered as part of recommendation development: 1) Essentiality, 2) Human Rights, and 3) Quality of the Evidence. It also includes three core Criteria that guide the development of a specific recommendation, informed by an evaluation of relevant evidence: 1) Environmental Justice, 2) Maximizing Benefits and Reducing Harm, and 3) Sociocultural Acceptability and Feasibility. The framework’s goal is to make the decision process transparent and comprehensive through explicit consideration of core factors important for decisions, leading to more equitable and health-protective interventions.
{"title":"Development of the Navigation Guide Evidence-to-Decision Framework for Environmental Health: Version 1.0","authors":"Nicholas Chartres, Max T. Aung, Susan L. Norris, Courtney Cooper, Lisa A. Bero, Roger Chou, Devon C. Payne-Sturges, Wendy E. Wagner, Jessica W. Reyes, Lisa M. Askie, Daniel A. Axelrad, Deysi Flores Vigo, Jill E. Johnston, Juleen Lam, Keeve E. Nachman, Eva Rehfuess, Rachel Rothschild, Patrice Sutton, Lauren Zeise, Tracey J. Woodruff","doi":"10.1021/acs.est.4c08063","DOIUrl":"https://doi.org/10.1021/acs.est.4c08063","url":null,"abstract":"Environmental exposures, including widespread industrial pollution, impact human health and are amplified in more highly exposed communities. Policy and regulatory frameworks for making decisions and recommendations on interventions to mitigate or prevent exposures tend to narrowly focus on exposure and some health-related data related to risks. Typically, such frameworks do not consider other factors, including essentiality, health equity, and distribution of benefits and costs. Further, decisions and recommendations lack transparency regarding how they were developed. We developed the Navigation Guide Evidence-to-Decision Framework for Environmental Health (E2DFEH) to provide a structured and transparent framework incorporating a range of scientific information and factors for decision-making. We reviewed current evidence-to-decision frameworks and engaged in an iterative consensus-based process involving 30 experts from 25 organizations in the academic, government, and nonprofit sectors. The E2DFEH framework includes three Foundations that are structural factors considered as part of recommendation development: 1) Essentiality, 2) Human Rights, and 3) Quality of the Evidence. It also includes three core Criteria that guide the development of a specific recommendation, informed by an evaluation of relevant evidence: 1) Environmental Justice, 2) Maximizing Benefits and Reducing Harm, and 3) Sociocultural Acceptability and Feasibility. The framework’s goal is to make the decision process transparent and comprehensive through explicit consideration of core factors important for decisions, leading to more equitable and health-protective interventions.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"1 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-02-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143507249","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-02-25Epub Date: 2025-02-13DOI: 10.1021/acs.est.4c09334
Geng Li, Peng Xu, Zhonghua Zheng, Jimmy C H Fung
Nitrogen oxides (NOx) play an important role in the formation of tropospheric ozone and fine particulate matter. Although regulatory policies in Southeast Asia have successfully limited combustion sources of NOx emissions, fertilized cropland NOx emissions have become increasingly prominent. However, the amount and geographic distribution of NOx emissions from fertilized croplands over Southeast Asia remain largely uncertain. Here, we use a bottom-up spatial model that combines temperature dependence and the Yienger and Levy (YL95) scheme to quantify the spatiotemporal changes in crop-specific fertilized cropland NOx emissions at five-arcminute resolution (about 10 km) from 1980 to 2019. The results show a 4-fold increase in NOx emissions from fertilized croplands in Southeast Asia from 12.9 Gg N yr-1 (R50, the difference between the 25% and 75% quantiles: 8.8-17.7 Gg N yr-1) in 1980 to 53.3 Gg N yr-1 (R50: 35.6-72.0 Gg N yr-1) in 2019. During 1980-2019, the annual NOx emissions of rice, maize and other crops showed increasing spatial trends (0.20, 0.21, and 0.63 Gg N yr-2, respectively), whereas those of wheat remained flat (-0.0006 Gg N yr-2). Our new estimate averages 19% lower than previous bottom-up and top-down estimates. The NOx emissions hotspots are mainly located in Indonesia, Vietnam, Thailand and the Philippines for rice, maize and other crops and in Myanmar for wheat. Our crop-specific and spatially explicit NOx emissions inventories can contribute to identifying emissions and reduction hotspots and assessing future policy implications regarding mitigation options for improving air quality and food security in Southeast Asia. Future studies that comprehensively consider meteorological conditions, soil properties, management practices and small-scale land-use changes can potentially lower the uncertainty of this estimation.
{"title":"Improved Crop-specific NOx Emissions from Croplands in Southeast Asia over 1980-2019.","authors":"Geng Li, Peng Xu, Zhonghua Zheng, Jimmy C H Fung","doi":"10.1021/acs.est.4c09334","DOIUrl":"10.1021/acs.est.4c09334","url":null,"abstract":"<p><p>Nitrogen oxides (NOx) play an important role in the formation of tropospheric ozone and fine particulate matter. Although regulatory policies in Southeast Asia have successfully limited combustion sources of NOx emissions, fertilized cropland NOx emissions have become increasingly prominent. However, the amount and geographic distribution of NOx emissions from fertilized croplands over Southeast Asia remain largely uncertain. Here, we use a bottom-up spatial model that combines temperature dependence and the Yienger and Levy (YL95) scheme to quantify the spatiotemporal changes in crop-specific fertilized cropland NOx emissions at five-arcminute resolution (about 10 km) from 1980 to 2019. The results show a 4-fold increase in NOx emissions from fertilized croplands in Southeast Asia from 12.9 Gg N yr<sup>-1</sup> (<i>R</i><sub>50</sub>, the difference between the 25% and 75% quantiles: 8.8-17.7 Gg N yr<sup>-1</sup>) in 1980 to 53.3 Gg N yr<sup>-1</sup> (<i>R</i><sub>50</sub>: 35.6-72.0 Gg N yr<sup>-1</sup>) in 2019. During 1980-2019, the annual NOx emissions of rice, maize and other crops showed increasing spatial trends (0.20, 0.21, and 0.63 Gg N yr<sup>-2</sup>, respectively), whereas those of wheat remained flat (-0.0006 Gg N yr<sup>-2</sup>). Our new estimate averages 19% lower than previous bottom-up and top-down estimates. The NOx emissions hotspots are mainly located in Indonesia, Vietnam, Thailand and the Philippines for rice, maize and other crops and in Myanmar for wheat. Our crop-specific and spatially explicit NOx emissions inventories can contribute to identifying emissions and reduction hotspots and assessing future policy implications regarding mitigation options for improving air quality and food security in Southeast Asia. Future studies that comprehensively consider meteorological conditions, soil properties, management practices and small-scale land-use changes can potentially lower the uncertainty of this estimation.</p>","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":" ","pages":"3562-3568"},"PeriodicalIF":10.8,"publicationDate":"2025-02-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143412290","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}
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