IF 9.028 1区环境科学与生态学

环境科学与技术 Pub Date : 2025-06-18 DOI: 10.1021/acs.est.4c13931

Yu Ting Zhang, Ana Gouveia, Ruanni Chen, Daochao Xing, Juying Wang, Jingli Mu

{"title":"Biomicroplastics and Antibiotics: A Toxic Cocktail for Fatty Liver Disease in Marine Medaka","authors":"Yu Ting Zhang, Ana Gouveia, Ruanni Chen, Daochao Xing, Juying Wang, Jingli Mu","doi":"10.1021/acs.est.4c13931","DOIUrl":"https://doi.org/10.1021/acs.est.4c13931","url":null,"abstract":"The increasing production and use of bioplastics contribute to the accumulation of bioplastic debris in marine environments. The impact of such debris, particularly when combined with co-occurring pollutants like antibiotics, on marine life remains largely unexplored. In this study, we demonstrate that coexposure to aged polylactic acid (PLA) biomicroplastics and the antibiotic sulfamethazine (SMZ) induces overweight (an increase of 20.9–26.2%) and fatty liver-like disease in juvenile marine medaka (Oryzias melastigma). We investigated the underlying mechanism involving the orchestration of physiological processes between the host and its gut microbiota. We found that SMZ acted as a precondition or driver, while PLA acted as an environmental selective pressure, directionally shaping the gut microbiota communities. This altered microbiota demonstrated an increased ability to break down PLA into lactic acid, activating intestinal gluconeogenesis and consequently generating glucose. Excessive glucose shifted the hepatic glucose-fat balance toward fat accumulation, resulting in triglyceride and lipid droplet accumulation and overweight in the fish. Given the prevalent co-occurrence and interaction of PLA and antibiotics in the real-world environment, the combined ecological risk posed by these pollutants requires further investigation.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"603 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-06-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144312042","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

Settling Velocities of Tire and Road Wear Particles: Analyzing Finely Graded Density Fractions of Samples from a Road Simulator and a Highway Tunnel 轮胎和道路磨损颗粒的沉降速度：分析公路模拟器和公路隧道样品的精细分级密度分数

IF 9.028 1区环境科学与生态学

环境科学与技术 Pub Date : 2025-06-18 DOI: 10.1021/acs.est.5c04165

Stefan Dittmar, Steffen Weyrauch, Thorsten Reemtsma, Paul Eisentraut, Korinna Altmann, Aki S. Ruhl, Martin Jekel

{"title":"Settling Velocities of Tire and Road Wear Particles: Analyzing Finely Graded Density Fractions of Samples from a Road Simulator and a Highway Tunnel","authors":"Stefan Dittmar, Steffen Weyrauch, Thorsten Reemtsma, Paul Eisentraut, Korinna Altmann, Aki S. Ruhl, Martin Jekel","doi":"10.1021/acs.est.5c04165","DOIUrl":"https://doi.org/10.1021/acs.est.5c04165","url":null,"abstract":"The terminal settling velocity is considered the most critical parameter determining the transport of tire and road wear particles (TRWP) in aquatic environments. Nonetheless, no respective empirical data has been reported so far. In this study, particle samples from a road simulator and a highway tunnel were investigated with a validated imaging method. Different density and size fractions of both samples were measured separately, acquiring sizes and settling velocities of more than 30,000 individual particles. In addition, tire marker polymers were analyzed for each fraction via thermal extraction desorption-gas chromatography/mass spectrometry. Finally, the acquired particle data was combined according to the fractions’ estimated tire contents in order to deduce detailed probability distributions of particle size and settling velocity for the actual TRWP from both samples. Weighted by TRWP-incorporated tire mass, median diameters of 54 and 44 μm as well as median settling velocities of 0.65 and 0.22 mm/s were found for TRWP from the road simulator and highway tunnel, respectively. This study thus provides the first ever empirical data on TRWP settling velocities in water, which can be highly valuable input for modeling the environmental transport of TRWP and for dimensioning TRWP retention systems.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"44 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-06-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144312043","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

Changes in the Temporal Targeting of the U.S. National Ambient Air Quality Standards (NAAQS) for SO2 Reduce Average and Peak Emissions from Coal Power Plants 美国国家环境空气质量标准（NAAQS）二氧化硫时间目标的变化减少了燃煤电厂的平均和峰值排放量

IF 9.028 1区环境科学与生态学

环境科学与技术 Pub Date : 2025-06-18 DOI: 10.1021/acs.est.4c10718

Joanna H. Slusarewicz, Valerie J. Karplus

{"title":"Changes in the Temporal Targeting of the U.S. National Ambient Air Quality Standards (NAAQS) for SO2 Reduce Average and Peak Emissions from Coal Power Plants","authors":"Joanna H. Slusarewicz, Valerie J. Karplus","doi":"10.1021/acs.est.4c10718","DOIUrl":"https://doi.org/10.1021/acs.est.4c10718","url":null,"abstract":"The U.S. National Ambient Air Quality Standards (NAAQS) protect public health by limiting ambient pollutant concentrations, but effects at power plants are not well characterized. We estimate how a 2010 SO2 NAAQS change that altered policy targeting from peak hourly emissions to annually aggregated hourly emissions affected SO2 emissions from coal-fired power plants. Using data on electricity generating unit (EGU) characteristics, SO2 emissions, fuel prices, and PM2.5 NAAQS classifications from 2001 to 2019 from public data sources, we estimate that, after a county was classified under the 2010 SO2 standard, EGUs reduced SO2 emissions during daily maximum hours by 31.6% (95% CI [−0.381, −0.247]) at the 99th percentile and 34.4% (95% CI [−0.424, −0.253]) at the 50th percentile. After a nearby ambient SO2 monitor was added to assess NAAQS compliance, hourly emissions fell by 12.4% (95% CI [−0.188, −0.054]) at the 99th percentile and 14.4% (95% CI [−0.228, −0.050]) at the 50th percentile. Our results also suggest the new standard had the same effect on peak hourly SO2 emissions as median and that plants in counties prioritized for early designation were less responsive to the policy change. These results suggest that the 2010 SO2 NAAQS change may have reduced SO2 emissions but may not have had an outsized impact on peak emissions despite policy guidance encouraging their control.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"34 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-06-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144312041","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

In Situ-Formed Tridentate Pd-SOx Coordination for Sulfur-Tolerant CO Oxidation Catalysis. 原位形成的三叉戟Pd-SOx配位在耐硫CO氧化催化中的应用。

IF 9.028 1区环境科学与生态学

环境科学与技术 Pub Date : 2025-06-18 DOI: 10.1021/acs.est.5c03547

Li Xiang,Chunqi Wang,Guo Nie,Menghe Lou,Xueqing Luo,Junying Ding,Renna Li,Zhongbiao Wu,Xiaole Weng

{"title":"In Situ-Formed Tridentate Pd-SOx Coordination for Sulfur-Tolerant CO Oxidation Catalysis.","authors":"Li Xiang,Chunqi Wang,Guo Nie,Menghe Lou,Xueqing Luo,Junying Ding,Renna Li,Zhongbiao Wu,Xiaole Weng","doi":"10.1021/acs.est.5c03547","DOIUrl":"https://doi.org/10.1021/acs.est.5c03547","url":null,"abstract":"SO2 impurity, widely existing in industrial exhaust, is a typical deactivator in many catalytic reactions. The poisoning mechanism of SO2 on the active sites of catalysts has been well acknowledged, yet the role of support in sulfur-tolerant catalysis remains elusive. Herein, TiO2, Al2O3, and CeO2 carriers were selected to unveil the sulfur resistance mechanism of Pd-based catalysts in catalytic CO oxidation. We showed that Pd/TiO2 effectively terminated continuous sulfidation, achieving 100% CO conversion at 175 °C for 200 h under SO2 and H2O exposure. This exceptional sulfur tolerance was attributed to the formation of a distinct tridentate sulfate structure on the PdO nanoparticles, facilitated by the moderate reducibility and strong acidity of Pd/TiO2. In contrast, Pd/Al2O3 and Pd/CeO2 remained only ∼70 and 5% efficiency, accompanied by the abundant formation of Pd-related bidentate and Ce-related tridentate sulfate species, respectively. Combined experimental and theoretical analyses revealed the distinct in situ-formed tridentate Pd-SOx coordination over Pd/TiO2 regulated the local electronic distribution, effectively mitigating the affinity of the catalyst to SO2 while preserving the redox capability and reactivity of oxygen species. Our findings are crucial for advancing sulfur-tolerant catalysis, offering valuable strategies for rationally designing robust catalysts to overcome both economic and environmental challenges in industrial applications.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"8 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-06-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144311370","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

Developing a Rate Law for Ce(III) Oxidation by Manganese Oxides. 锰氧化物氧化Ce（III）的速率规律。

IF 9.028 1区环境科学与生态学

环境科学与技术 Pub Date : 2025-06-17 DOI: 10.1021/acs.est.4c12688

Hang Xu,Pan Liu,Simin Zhao,Yinghao Wen,Yuanzhi Tang

{"title":"Developing a Rate Law for Ce(III) Oxidation by Manganese Oxides.","authors":"Hang Xu,Pan Liu,Simin Zhao,Yinghao Wen,Yuanzhi Tang","doi":"10.1021/acs.est.4c12688","DOIUrl":"https://doi.org/10.1021/acs.est.4c12688","url":null,"abstract":"Rare earth elements (REEs) are critical minerals that are indispensable for clean energy technologies. Understanding REE occurrence and transport in natural environments is important for the prediction and identification of REE resources. Cerium (Ce) is a rare earth element that exhibits multiple oxidation states. The oxidation of dissolved Ce(III) by manganese oxides (MnO2) and the resulting Ce anomaly is used as an indicator for tracing biogeochemical processes controlling REE transport and mobility, as well as a paleo-redox proxy for understanding Earth's oxygenation events. However, a detailed kinetic rate law for this process is still lacking. This study determines the reaction orders and rate constant for Ce(III) oxidation by δ-MnO2 using the initial rate method. The overall reaction follows a first order for Ce(III) and δ-MnO2 and a 0.5th order for OH-, resulting in an overall 2.5th order. The calculated overall rate constant (k) was 1.4 × 106 L3/2 mol-1/2 g-1 h-1. Kinetic modeling was employed to distinguish Ce adsorption and oxidation by using redox-inert Ce-analogues La and Nd. Our experimental and kinetic modeling results suggest that Ce(III) oxidation by δ-MnO2 occurs in multiple steps: the adsorption of Ce(III) on the δ-MnO2 surface, the oxidation of Ce(III), and surface precipitation of CeIVO2. Our findings provide important insights into the quantitative applications of Ce anomaly as a proxy to investigate various biogeochemical processes.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"145 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-06-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144311490","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

Pore-Size-Dependent Kinetics and Product Distribution of Fe(II)-Catalyzed Ferrihydrite Transformation. 铁（II）催化水合铁转化的孔径依赖性动力学和产物分布。

IF 9.028 1区环境科学与生态学

环境科学与技术 Pub Date : 2025-06-17 DOI: 10.1021/acs.est.5c03094

Linxin Cheng,Yuefei Ding,Yuanyuan Liu,Jing Chen,Xiaohui Wu,Juan Liu,Linling Wang,Anxu Sheng

{"title":"Pore-Size-Dependent Kinetics and Product Distribution of Fe(II)-Catalyzed Ferrihydrite Transformation.","authors":"Linxin Cheng,Yuefei Ding,Yuanyuan Liu,Jing Chen,Xiaohui Wu,Juan Liu,Linling Wang,Anxu Sheng","doi":"10.1021/acs.est.5c03094","DOIUrl":"https://doi.org/10.1021/acs.est.5c03094","url":null,"abstract":"Fe(II)-catalyzed ferrihydrite (Fh) transformation is a widely occurring biogeochemical process in the porous media of anaerobic soils and sediments, but how pore-scale spaces affect the kinetics and product distribution of Fh transformation remains poorly understood. This study investigated the transformation of Fh nanoparticle film across a continuum of sizes of pore-scale spaces created by pressing a glass bead onto the film and immersing in 2 mM and 10 mM FeSO4 at pH = 7.0. While lepidocrocite (Lp) dominated over goethite (Gt) on the static Fh film, both minerals were observed to preferentially precipitate in micropore regions adjacent to the Fh film-glass bead contact area. The natural logarithm of product formation rates decreased linearly as increasing pore height (h) from 5 to 600 μm, revealing pronounced kinetic inhibition in macropore regions. Product mineral particles in smaller pore regions exhibited reduced primary particle size (146.1 ± 57.6 nm at h = 0.11 μm) compared with those in larger pores (222.5 ± 61.8 nm at h = 561.84 μm). COMSOL-based reaction-diffusion modeling shows that rapid Fe(III)labile intermediate supply from Fe(II)-catalyzed Fh dissolution drives its localized accumulation and elevated supersaturation within confined micropores, which ultimately dictates the pore-size-dependent distribution, formation kinetics, and primary particle size of the resulting product minerals. These findings provide mechanistic insights into the dominant role of intermediate precursor supply in dictating confinement-regulated phase transformation and highlight the notable effects of micropore size on Fh transformation and element cycling in natural porous media.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"14 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-06-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144311497","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

Blood-Brain and Blood-Gill Barrier Disruption in Coho Salmon Exposed to Roadway Runoff and 6PPD-Quinone. 暴露于道路径流和6ppd -醌的银鲑血脑和血鳃屏障破坏。

IF 9.028 1区环境科学与生态学

环境科学与技术 Pub Date : 2025-06-17 DOI: 10.1021/acs.est.5c01559

Stephanie I Blair,Jill Wetzel,Melissa Gonzalez,Edward P Kolodziej,Chelsea J Mitchell,Garrett M Foster,Valerie Lynch-Holm,Jenifer K McIntyre

{"title":"Blood-Brain and Blood-Gill Barrier Disruption in Coho Salmon Exposed to Roadway Runoff and 6PPD-Quinone.","authors":"Stephanie I Blair,Jill Wetzel,Melissa Gonzalez,Edward P Kolodziej,Chelsea J Mitchell,Garrett M Foster,Valerie Lynch-Holm,Jenifer K McIntyre","doi":"10.1021/acs.est.5c01559","DOIUrl":"https://doi.org/10.1021/acs.est.5c01559","url":null,"abstract":"The tire-derived chemical N-(1,3-dimethylbutyl)-N'-phenyl-p-phenylenediamine-quinone (6PPD-quinone) causes acute mortality in coho salmon (Oncorhynchus kisutch), yet its mechanisms of toxicity remain poorly understood. We exposed juvenile coho salmon to roadway runoff or 6PPD-quinone to investigate whether disruption of the blood-brain barrier (BBB) and blood-gill barrier cause behavioral symptoms of urban runoff mortality syndrome in this sensitive species. BBB disruption was present in one-third of presymptomatic fish and in all symptomatic individuals, supporting its role in toxicity. Co-occurring brain and gill barrier disruptions at the onset of sustained surface swimming suggest a systemic vascular response rather than localized brain injury. Histological analysis of coho brains revealed red blood cell congestion within intact endothelia, consistent with circulatory collapse and plasma leakage, likely impairing oxygen delivery and disrupting neuronal signaling. Behavioral symptoms also coincided with altered expression of BBB junctional proteins genes (ocln, cld5α, and vecad). In Chinook salmon (Oncorhynchus tshawytscha), exposure to a high but environmentally relevant concentration of 6PPD-quinone reduced expression of the scaffolding protein zo-1, suggesting potential sublethal effects. These findings identify BBB disruption as a key event in 6PPD-quinone toxicity and link vascular injury to behavioral symptoms in coho salmon. Ongoing work in this model will further clarify mechanisms of action and support assessments of environmental and human health risks from tire-derived chemicals.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"26 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-06-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144311493","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

N-Acyl-Homoserine Lactone (AHL)-Mediated Initial Adhesion Behaviors of Bacteria onto Plastics. n -酰基-高丝氨酸内酯（AHL）介导的细菌对塑料的初始粘附行为。

IF 10.8 1区环境科学与生态学

环境科学与技术 Pub Date : 2025-06-17 DOI: 10.1021/acs.est.5c04426

Shuai Wang, Xiangyu Su, Jianmei Qin, Lei He, Meiping Tong

{"title":"N-Acyl-Homoserine Lactone (AHL)-Mediated Initial Adhesion Behaviors of Bacteria onto Plastics.","authors":"Shuai Wang, Xiangyu Su, Jianmei Qin, Lei He, Meiping Tong","doi":"10.1021/acs.est.5c04426","DOIUrl":"https://doi.org/10.1021/acs.est.5c04426","url":null,"abstract":"The initial adhesion of microbes onto plastics is crucial for the subsequent formation of the plastisphere, which might be affected by signal molecules commonly present in bacteria-related environments that regulate cell-to-cell communication. Herein, the initial retention performance of E. coli onto six types of plastics, both without and with N-acyl-homoserine lactones (AHLs, a common signal molecule) at concentrations ranging from 10 ng/L to 100 μg/L in suspension, was determined to reveal the influence of signal molecules on the formation of the plastisphere. We found that AHLs coexisting in suspensions significantly enhanced bacterial adhesion performance onto plastics, regardless of plastic types and AHL types, with a more pronounced enhancement observed at higher AHL concentrations. This enhanced bacterial adhesion induced by AHLs also held true in solutions containing humic acid, in river water, and in sewage. AHLs stimulated the synthesis of EPS, enhanced EPS hydrophobicity by altering the protein/polysaccharide ratio and its secondary structures, and upregulated pathways related to flagellar assembly, quorum sensing, protein production, and biofilm formation, thereby enhancing bacterial adhesion capability onto plastics. Moreover, AHLs adsorbed onto plastic surfaces could induce chemoattraction effects, further promoting bacterial adhesion performance. Obviously, through various mechanisms, the signal molecules greatly influence the initial adhesion of bacteria onto plastics in aquatic systems.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":" ","pages":""},"PeriodicalIF":10.8,"publicationDate":"2025-06-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144309252","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

Nontargeted Analysis of Surface and Groundwaters Impacted by Historic PFAS Waste Sites. 受历史PFAS废料场影响的地表水和地下水的非目标分析。

IF 9.028 1区环境科学与生态学

环境科学与技术 Pub Date : 2025-06-17 DOI: 10.1021/acs.est.5c03243

Heather D Whitehead,Timothy J Buckley,Jon R Sobus,Jacqueline Bangma,Denise K MacMillan,Antony J Williams,Gregory Janesch,James Coombs,Erin Newman,Andri Dahlmeier,Stefan Saravia,Rosie Rushing,Marla DeVault,James P McCord

{"title":"Nontargeted Analysis of Surface and Groundwaters Impacted by Historic PFAS Waste Sites.","authors":"Heather D Whitehead,Timothy J Buckley,Jon R Sobus,Jacqueline Bangma,Denise K MacMillan,Antony J Williams,Gregory Janesch,James Coombs,Erin Newman,Andri Dahlmeier,Stefan Saravia,Rosie Rushing,Marla DeVault,James P McCord","doi":"10.1021/acs.est.5c03243","DOIUrl":"https://doi.org/10.1021/acs.est.5c03243","url":null,"abstract":"Per- and polyfluoroalkyl substances (PFAS) make up a diverse class of anthropogenic chemicals with widespread industrial and commercial uses. Historical manufacturing and disposal of PFAS have led to their introduction to the environment, although only a fraction of existing PFAS are routinely monitored using targeted analysis methods. Here, nontargeted analysis was used to investigate the identity and fate of PFAS present in eight groundwater and nine surface water samples collected near St. Paul, MN, surrounding two sites that historically received wastes from a PFAS manufacturer in the 1940-1970s. A total of 210 PFAS, split across 33 different homologous series, were identified in surface and groundwater samples both at and downstream of the two waste sites. Identified compounds included perfluorinated, polyfluorinated, and unsaturated sulfonic and carboxylic acid species as well as a variety of sulfonamide and sulfonamido chemistries. PFAS measured downgradient included legacy perfluorinated sulfonic and carboxylic acids, as well as their polyfluorinated, unsaturated, keto, and ether-containing analogs. Two-thirds of the identified PFAS were unique to the groundwater at one site. The lack of these PFAS at downstream sites likely reflects dilution below the limit of detection during downgradient transport. The identified species reveal previously unknown and substantial ongoing contamination of the watershed due to historic PFAS manufacturing and waste disposal.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"36 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-06-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144311488","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

Accurate Quantification of Multifunctional C2-3 Organosulfates in Atmospheric Aerosols Using Liquid Chromatography-Electrospray Ionization Mass Spectrometry: Overcoming Matrix Effects and Underestimation. 使用液相色谱-电喷雾电离质谱法精确定量大气气溶胶中多功能co2 -3有机硫酸盐：克服基质效应和低估。

IF 9.028 1区环境科学与生态学

环境科学与技术 Pub Date : 2025-06-17 DOI: 10.1021/acs.est.5c01846

Shumin Liang,Yuchen Wang,Hanzhe Chen,Wan Chan,Jian Zhen Yu

{"title":"Accurate Quantification of Multifunctional C2-3 Organosulfates in Atmospheric Aerosols Using Liquid Chromatography-Electrospray Ionization Mass Spectrometry: Overcoming Matrix Effects and Underestimation.","authors":"Shumin Liang,Yuchen Wang,Hanzhe Chen,Wan Chan,Jian Zhen Yu","doi":"10.1021/acs.est.5c01846","DOIUrl":"https://doi.org/10.1021/acs.est.5c01846","url":null,"abstract":"Reversed-phase liquid chromatography (RPLC) coupled with electrospray ionization-mass spectrometry (ESI-MS) is widely used to analyze polar organic compounds in atmospheric particulate matter (PM). However, its efficacy for small, polar multifunctional C2-C3 organosulfates (C2-3OSs)─conceivably key products of isoprene oxidation─is questionable. Notable matrix effects are anticipated to arise from poor retention and coelution with abundant salts in PM samples. Here, we systematically evaluated RPLC versus hydrophilic interaction liquid chromatography (HILIC) coupled with ESI-Orbitrap MS in quantifying PM-bound C2-3OSs. We synthesized three C2-3OSs, including glycolic acid sulfate, hydroxyacetone sulfate, and lactic acid sulfate. The availability of authentic standards enabled the first quantitative assessment of measurement bias for C2-3OSs using the RPLC-ESI-Orbitrap MS method, revealing an underestimation of these compounds by 1-2 orders of magnitude. The measurement bias primarily stemmed from the matrix effects arising from the coexisting bisulfate in ambient PM. In contrast, HILIC notably outperformed RPLC in retentive capacities and peak resolving abilities, effectively avoiding matrix suppression effects. Additionally, the HILIC-ESI-MS method uncovered six previously unreported C2-3OSs, expanding our knowledge of atmospheric OSs. This work enhances our capability of accurate quantification of aerosol components, thus helping to reduce constraints on studies of aerosols and their impacts.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"39 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2025-06-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144311494","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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