Environmental Science & Technology Letters Environ.最新文献

筛选
英文 中文
Occurrence of the Tire-Derived Toxicant 6PPD-Quinone in Road Dust from Unpaved Roads in a Cold-Region Urban Area 寒冷地区城市道路粉尘中轮胎源毒物6ppd -醌的发生
IF 8.8 2区 环境科学与生态学
Environmental Science & Technology Letters Environ. Pub Date : 2025-08-19 DOI: 10.1021/acs.estlett.5c00726
Leland T. Bryshun, Blake Hunnie, Kerry N. McPhedran and Markus Brinkmann*, 
{"title":"Occurrence of the Tire-Derived Toxicant 6PPD-Quinone in Road Dust from Unpaved Roads in a Cold-Region Urban Area","authors":"Leland T. Bryshun,&nbsp;Blake Hunnie,&nbsp;Kerry N. McPhedran and Markus Brinkmann*,&nbsp;","doi":"10.1021/acs.estlett.5c00726","DOIUrl":"https://doi.org/10.1021/acs.estlett.5c00726","url":null,"abstract":"<p >In 2021, mortalities of coho salmon were linked to 6PPD-quinone (6PPD-Q), a transformation product formed from an antioxidant in rubber tires. Since then, research concerning 6PPD-Q contamination pathways has focused on paved roads. However, over half of the road network in Canada consists of unpaved roads, which remain unstudied for 6PPD-Q contamination. In this paper, we hypothesize that (1) unpaved road networks can provide a pathway for 6PPD-Q to enter the environment and (2) 6PPD-Q concentrations in unpaved road dust are influenced by location, speed limit, collection date, and total organic carbon (TOC) content of the roads. To investigate this, we collected gravel from the surface of unpaved roads in and around Saskatoon, Saskatchewan, Canada. Chemical extractions of road dust allowed for the detection and quantification of 6PPD-Q within each sample. Concentrations of 6PPD-Q ranged between 0.207 and 1.47 ng/g of dw (median: 0.511 ng/g of dw). When normalized to TOC content, concentrations varied between 9.83 and 342 ng/g of TOC (median: 145 ng/g of TOC). No factor other than the speed limit showed a positive linear relationship with 6PPD-Q concentrations. The results of this study are an initial glimpse into the role unpaved roads play in adding 6PPD-Q into the environment.</p>","PeriodicalId":37,"journal":{"name":"Environmental Science & Technology Letters Environ.","volume":"12 9","pages":"1247–1251"},"PeriodicalIF":8.8,"publicationDate":"2025-08-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145009533","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
Building Collision Fatalities for Monitoring Per- and Polyfluorinated Alkyl Substances (PFAS) in Wild Bird Populations 监测野生鸟类种群中全氟和多氟烷基物质(PFAS)的建筑物碰撞死亡率
IF 8.8 2区 环境科学与生态学
Environmental Science & Technology Letters Environ. Pub Date : 2025-08-18 DOI: 10.1021/acs.estlett.5c00676
Gordon J. Getzinger*,  and , Ben D. Marks, 
{"title":"Building Collision Fatalities for Monitoring Per- and Polyfluorinated Alkyl Substances (PFAS) in Wild Bird Populations","authors":"Gordon J. Getzinger*,&nbsp; and ,&nbsp;Ben D. Marks,&nbsp;","doi":"10.1021/acs.estlett.5c00676","DOIUrl":"https://doi.org/10.1021/acs.estlett.5c00676","url":null,"abstract":"<p >Ecosystem exposures and effects of per- and polyfluoroalkyl substances (PFAS) are poorly understood. Field studies reveal that birds bioaccumulate PFAS through ecosystem exposures. However, drivers of PFAS exposures are poorly understood and may suffer from species and geographic biases due to the significant effort and cost of conducting field studies for measuring PFAS in wild birds. Therefore, alternative methods for assessing avian PFAS exposures are needed. Herein, we explore the utility of opportunistic sampling of building collision fatalities for expanding knowledge of PFAS exposures in wild birds. Concentrations of 40 PFAS of regulatory concern were measured in 50 livers from eight passerine species killed in building strikes during their migration through Chicago, IL. Results indicate that exposure is dominated by perfluoroalkyl carboxylic acids, fluorotelomer carboxylic acids, and perfluoroalkyl sulfonic acids and that physiological factors and feeding strategies may impact PFAS exposures. Comparing liver concentrations to those found in similar species at contaminated and noncontaminated sites indicates that PFAS levels detected in building collision fatalities are representative of levels found in wild populations, suggesting that this approach may circumvent challenges encountered in traditional bird biomonitoring studies and offer opportunities for more detailed study of factors governing PFAS exposure and bioaccumulation.</p>","PeriodicalId":37,"journal":{"name":"Environmental Science & Technology Letters Environ.","volume":"12 9","pages":"1232–1237"},"PeriodicalIF":8.8,"publicationDate":"2025-08-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145009742","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
A Novel Chemical-Space-Dependent Strategy for Compound Selection in Non-target LC-HRMS Method Development Using Physicochemical and Structural Data 基于物理化学和结构数据的非目标LC-HRMS方法中化合物选择的新化学空间依赖策略
IF 8.8 2区 环境科学与生态学
Environmental Science & Technology Letters Environ. Pub Date : 2025-08-18 DOI: 10.1021/acs.estlett.5c00759
Lapo Renai*, Viktoriia Turkina, Tobias Hulleman, Alexandros Nikolopoulos, Andrea F. G. Gargano, Elvio D. Amato, Massimo Del Bubba and Saer Samanipour*, 
{"title":"A Novel Chemical-Space-Dependent Strategy for Compound Selection in Non-target LC-HRMS Method Development Using Physicochemical and Structural Data","authors":"Lapo Renai*,&nbsp;Viktoriia Turkina,&nbsp;Tobias Hulleman,&nbsp;Alexandros Nikolopoulos,&nbsp;Andrea F. G. Gargano,&nbsp;Elvio D. Amato,&nbsp;Massimo Del Bubba and Saer Samanipour*,&nbsp;","doi":"10.1021/acs.estlett.5c00759","DOIUrl":"https://doi.org/10.1021/acs.estlett.5c00759","url":null,"abstract":"<p >The virtual chemical space of substances, including emerging contaminants relevant to the environment and exposome, is rapidly expanding. Non-targeted analysis (NTA) by liquid chromatography–high-resolution mass spectrometry (LC-HRMS) is useful in measuring broad chemical space regions. Internal standards are typically used to optimize the selectivity and sensitivity of NTA LC-HRMS methods, assuming a linear relationship between structure and behavior across all analytes. However, this assumption fails for large, heterogeneous chemical spaces, narrowing measurable coverage to structurally similar compounds. We present a data-driven strategy for unbiased sampling of candidate structures for NTA LC-HRMS method development from extensive chemical spaces, such as the U.S. EPA’s CompTox (&gt;1 million chemicals). The workflow maximizes physicochemical/structural diversity using precomputed PubChem descriptors (e.g., molecular weight, XLogP) and grants LC-HRMS compatibility thanks to predicted mobility and ionization efficiency from molecular fingerprints. The resulting measurable compound lists (MCLs) provide broad, heterogeneous coverage for NTA method development, validation, and boundary assessment. Applied to the CompTox space, the approach yielded MCLs with greater chemical coverage and broader predicted LC-HRMS applicability than conventional “watch list” contaminants, offering a robust framework for enhancing NTA’s measurable chemical space while preserving diversity.</p>","PeriodicalId":37,"journal":{"name":"Environmental Science & Technology Letters Environ.","volume":"12 9","pages":"1162–1168"},"PeriodicalIF":8.8,"publicationDate":"2025-08-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acs.estlett.5c00759","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145009715","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Chemically Induced Decline in Wintertime SO2 Emission Control Efficacy 化学诱导的冬季SO2排放控制效果下降
IF 8.8 2区 环境科学与生态学
Environmental Science & Technology Letters Environ. Pub Date : 2025-08-18 DOI: 10.1021/acs.estlett.5c00731
Fanghe Zhao, Yuhang Wang* and Shengjun Xi, 
{"title":"Chemically Induced Decline in Wintertime SO2 Emission Control Efficacy","authors":"Fanghe Zhao,&nbsp;Yuhang Wang* and Shengjun Xi,&nbsp;","doi":"10.1021/acs.estlett.5c00731","DOIUrl":"https://doi.org/10.1021/acs.estlett.5c00731","url":null,"abstract":"<p >The reduction of SO<sub>2</sub> emissions from 2004 to 2023 has resulted in significant decreases in SO<sub>2</sub> and sulfate concentrations across the Rust Belt and Southeast of the United States, regions with coal-combustion power plant emissions. While the observed sulfate-to-total-sulfur ratio remained relatively constant at ∼30% in summer, this fraction increased from ∼10% to ∼20% in winter from 2004 to 2013 and then remained at ∼20%. The rise in sulfate-to-total-sulfur ratio resulted in a slower decrease of sulfate in 2004–2013 compared to 2013–2023 despite a greater reduction of SO<sub>2</sub> in the earlier decade, reflecting a significant decline in the efficacy of SO<sub>2</sub> emission reduction in improving air quality in winter. The decrease in efficacy is attributed to the increased oxidation of SO<sub>2</sub> in winter because of the diminishing oversupply of SO<sub>2</sub> compared to the availability of atmospheric oxidant, H<sub>2</sub>O<sub>2</sub>. Consequently, the seasonal differences in SO<sub>2</sub> and sulfate concentrations between summer and winter have narrowed. This chemical damping effect, caused by limited oxidant availability, is likely to delay the reduction in sulfate concentrations in other polluted regions where the transition from coal to natural gas in power plants or alternative energy sources has not progressed as rapidly as in the United States.</p>","PeriodicalId":37,"journal":{"name":"Environmental Science & Technology Letters Environ.","volume":"12 9","pages":"1190–1196"},"PeriodicalIF":8.8,"publicationDate":"2025-08-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acs.estlett.5c00731","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145009714","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Rapid and Selective Recovery of Boron from Desalination Waste Using N-Methyl-d-glucamine-Modified Bioadsorbent n -甲基-d-氨基葡萄糖改性生物吸附剂快速选择性回收海水淡化废水中的硼
IF 8.8 2区 环境科学与生态学
Environmental Science & Technology Letters Environ. Pub Date : 2025-08-18 DOI: 10.1021/acs.estlett.5c00645
Shoji Yoshioka, Yuma Ito, Tsuyoshi Taniguchi, Shafiqur Rahman*, Masaru Endo, Kuo H. Wong, Asami S. Mashio, Tatsuya Nishimura, Katsuhiro Maeda and Hiroshi Hasegawa*, 
{"title":"Rapid and Selective Recovery of Boron from Desalination Waste Using N-Methyl-d-glucamine-Modified Bioadsorbent","authors":"Shoji Yoshioka,&nbsp;Yuma Ito,&nbsp;Tsuyoshi Taniguchi,&nbsp;Shafiqur Rahman*,&nbsp;Masaru Endo,&nbsp;Kuo H. Wong,&nbsp;Asami S. Mashio,&nbsp;Tatsuya Nishimura,&nbsp;Katsuhiro Maeda and Hiroshi Hasegawa*,&nbsp;","doi":"10.1021/acs.estlett.5c00645","DOIUrl":"https://doi.org/10.1021/acs.estlett.5c00645","url":null,"abstract":"<p >Recovering boron (B) from desalination brine is essential for sustainable resource management and meeting critical raw material demands. In this study, we designed and evaluated a novel bioadsorbent, <i>N</i>-methyl-<span>d</span>-glucamine (NMDG)-modified cellulose (MGMC), for selective B recovery from desalination brine. The adsorption kinetics, isotherms, selectivity, and influence of competing salts were examined, along with B recovery from seawater and simulated desalination brine. Fourier-transform infrared spectroscopy, X-ray photoelectron spectroscopy, and pH at the point of zero charge (pH<sub>PZC</sub>) analysis were used to elucidate the adsorption mechanism. MGMC attained rapid adsorption equilibrium within 0.5 h and exhibited a high B adsorption capacity of 1,647 μmol g<sup>–1</sup>, surpassing commercial adsorbents and most previously reported NMDG-modified derivatives. Moreover, MGMC demonstrated excellent selectivity for B, effectively rejecting diverse metals and oxyanions. Furthermore, it achieved ≥97% B sorption from seawater and simulated brine with shorter contact times and lower dosages than commercial resins. MGMC’s outstanding B selectivity is attributed to the strong coordinated interaction between B and the hydroxy groups in its NMDG-rich structure, further aided by a low pH<sub>PZC</sub> (6.9). Our findings demonstrate MGMC as a cost-effective and eco-friendly solution for selective B recovery from desalination processes, presenting a promising avenue for sustainable resource management.</p>","PeriodicalId":37,"journal":{"name":"Environmental Science & Technology Letters Environ.","volume":"12 9","pages":"1264–1270"},"PeriodicalIF":8.8,"publicationDate":"2025-08-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145009739","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
Recent Advances in Engineered MoS2-Based Nanomaterials for CO2 Electro-Reduction to CO and Beyond 基于二硫化钼的CO2电还原纳米材料的研究进展
IF 8.8 2区 环境科学与生态学
Environmental Science & Technology Letters Environ. Pub Date : 2025-08-15 DOI: 10.1021/acs.estlett.5c00465
Anirban Mukherjee, Niwesh Ojha*, Kamal Kishore Pant, Aniruddha Deb, Maryam Abdinejad*, Susanta Sinha Mahapatra* and Bidhan Chandra Ruidas*, 
{"title":"Recent Advances in Engineered MoS2-Based Nanomaterials for CO2 Electro-Reduction to CO and Beyond","authors":"Anirban Mukherjee,&nbsp;Niwesh Ojha*,&nbsp;Kamal Kishore Pant,&nbsp;Aniruddha Deb,&nbsp;Maryam Abdinejad*,&nbsp;Susanta Sinha Mahapatra* and Bidhan Chandra Ruidas*,&nbsp;","doi":"10.1021/acs.estlett.5c00465","DOIUrl":"https://doi.org/10.1021/acs.estlett.5c00465","url":null,"abstract":"<p >The conversion of carbon dioxide (CO<sub>2</sub>) into value-added compounds is an emerging climate-change mitigation technique. Among various approaches, electrochemical CO<sub>2</sub> reduction (ECO<sub>2</sub>R) driven by renewable energy sources is considered one of the most viable methods for CO<sub>2</sub> reduction. Thus, developing efficient, cost-effective electrocatalysts that enhance reaction kinetics is vital for advancing ECO<sub>2</sub>R and enabling large-scale implementation. During the past few years, among the several transition metal dichalcogenides, molybdenum disulfide (MoS<sub>2</sub>) has attracted much interest in the field of electrocatalysis owing to its two-dimensional (2D) structure and high density of active sites, which could lead to the development of several high-performance ECO<sub>2</sub>R catalysts. This review presents the development and design of MoS<sub>2</sub>-based nanomaterials tailored for electrochemical CO<sub>2</sub> reduction (ECO<sub>2</sub>R), exploring the relationship between engineering strategies, catalytic performance, CO<sub>2</sub> conversion efficiency, and reaction pathways, while also highlighting controlled synthesis methods, recent advances in catalyst design for active site stabilization, and the influence of electrolytes on ECO<sub>2</sub>R performance. It also underscores the significant challenges that need to be overcome for the real-world implementation of MoS<sub>2</sub>-based nanomaterials in ECO<sub>2</sub>R to produce value-added chemicals, emphasizing the need for further research and development in this area.</p>","PeriodicalId":37,"journal":{"name":"Environmental Science & Technology Letters Environ.","volume":"12 9","pages":"1113–1138"},"PeriodicalIF":8.8,"publicationDate":"2025-08-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145009671","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
Environmentally Persistent Free Radicals in Outdoor Surface Grime during Pollen Season 花粉季节室外表面尘垢的环境持久性自由基
IF 8.8 2区 环境科学与生态学
Environmental Science & Technology Letters Environ. Pub Date : 2025-08-15 DOI: 10.1021/acs.estlett.5c00319
Stephanie R. Schneider*, Amara L. Holder and Sarah A. Styler, 
{"title":"Environmentally Persistent Free Radicals in Outdoor Surface Grime during Pollen Season","authors":"Stephanie R. Schneider*,&nbsp;Amara L. Holder and Sarah A. Styler,&nbsp;","doi":"10.1021/acs.estlett.5c00319","DOIUrl":"https://doi.org/10.1021/acs.estlett.5c00319","url":null,"abstract":"<p >On outdoor surfaces, grime is an important substrate for the deposition and reactive loss of semivolatile and particulate bound pollutants. A previously unexplored source of grime reactivity is environmentally persistent free radicals (EPFRs), which are precursors to reactive oxygen species (ROS). To measure EPFRs in grime, grime was collected in Spring 2023 on glass beads deployed in suburban North Carolina, where possible primary EPFR sources include pollen and nearby prescribed burning. EPFRs are measured in all collected grime samples via electron paramagnetic resonance spectroscopy after extraction of the grime onto filters. Pollen contains the majority of the collected grime mass, and when isolated from the smaller component of the grime constituents via filtration, it comprises most of the measured EPFRs. Endogenous EPFRs were measured in commercial pollen samples (<i>Quercus rubra</i>, <i>Quercus velutina</i>, and <i>Betula pendula</i>), which supports the conclusion that pollen contributed to the overall EPFRs measured in the grime. Grime samples were collected under shaded conditions, which limits photochemistry as a secondary source of EPFRs in the field samples; to further investigate light mediated EPFR formation mechanisms, we also measured EPFRs in grime following laboratory photoaging. EPFRs are formed from irradiation in all grime samples; however, extended irradiation eventually reduces the number of EPFRs to their starting numbers, a trend which was also observed with the irradiation of the commercial pollen. The increase of EPFRs over grime age and with irradiation implies that ROS production in grime from EPFRs may also be sensitive to aging over time.</p>","PeriodicalId":37,"journal":{"name":"Environmental Science & Technology Letters Environ.","volume":"12 9","pages":"1211–1217"},"PeriodicalIF":8.8,"publicationDate":"2025-08-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145009681","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
Discrepancies between Personal and Ambient Temperatures at Hourly Scale: Insights from Wearable Sensors and Environmental Modeling 个人和环境温度在小时尺度上的差异:来自可穿戴传感器和环境建模的见解
IF 8.8 2区 环境科学与生态学
Environmental Science & Technology Letters Environ. Pub Date : 2025-08-15 DOI: 10.1021/acs.estlett.5c00672
Xin Meng, Minjung Lee, Lingzhi Chu, Soohyun Nam* and Kai Chen*, 
{"title":"Discrepancies between Personal and Ambient Temperatures at Hourly Scale: Insights from Wearable Sensors and Environmental Modeling","authors":"Xin Meng,&nbsp;Minjung Lee,&nbsp;Lingzhi Chu,&nbsp;Soohyun Nam* and Kai Chen*,&nbsp;","doi":"10.1021/acs.estlett.5c00672","DOIUrl":"https://doi.org/10.1021/acs.estlett.5c00672","url":null,"abstract":"<p >Accurate assessment of personal exposure to ambient temperature is essential for understanding temperature-related health impacts. However, the bias from using ambient temperature estimates as proxies for personal exposure remains underexplored, particularly on the hourly scale. This study integrated wearable temperature sensors with a high-resolution (1 km, hourly) ambient temperature model to evaluate individual-level ambient exposure among 94 individuals in Connecticut, USA, monitored across seasons between October 2023 and January 2025. Personal temperature was consistently higher than ambient temperature, with a larger difference during cooler months. The hourly difference exhibited a distinct unimodal diurnal pattern, smallest in the early afternoon. Linear mixed-effects models identified ambient temperature, hour of day, month, solar radiation, and the nightlight index as the key predictors of personal temperature and its deviation from ambient conditions. The temperature difference was well characterized by the model (marginal R<sup>2</sup> of 0.854). Extreme gradient boosting with SHapley Additive Explanations confirmed the ambient temperature and hour of day as the most influential features, with albedo and other environmental factors showing smaller effects. Findings highlight systematic seasonal and diurnal biases in ambient-based metrics, underscoring the need to account for these patterns in the assessment of thermal exposures.</p>","PeriodicalId":37,"journal":{"name":"Environmental Science & Technology Letters Environ.","volume":"12 9","pages":"1154–1161"},"PeriodicalIF":8.8,"publicationDate":"2025-08-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145009675","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
Discovery of Fluorotelomer Sulfones in the Blubber of Greenland Killer Whales (Orcinus orca) 格陵兰虎鲸(Orcinus orca)鲸脂中氟端聚体砜的发现
IF 8.8 2区 环境科学与生态学
Environmental Science & Technology Letters Environ. Pub Date : 2025-08-13 DOI: 10.1021/acs.estlett.5c00516
Mélanie Z. Lauria*, Xiaodi Shi, Faiz Haque, Merle Plassmann, Anna Roos, Malene Simon, Jonathan P. Benskin* and Karl J. Jobst*, 
{"title":"Discovery of Fluorotelomer Sulfones in the Blubber of Greenland Killer Whales (Orcinus orca)","authors":"Mélanie Z. Lauria*,&nbsp;Xiaodi Shi,&nbsp;Faiz Haque,&nbsp;Merle Plassmann,&nbsp;Anna Roos,&nbsp;Malene Simon,&nbsp;Jonathan P. Benskin* and Karl J. Jobst*,&nbsp;","doi":"10.1021/acs.estlett.5c00516","DOIUrl":"https://doi.org/10.1021/acs.estlett.5c00516","url":null,"abstract":"<p >Most known per- and polyfluoroalkyl substances (PFAS) bioaccumulate by binding to proteins or partitioning to phospholipids, leading to their prevalence in liver and blood. However, the recent discovery of high concentrations of unidentified extractable organofluorine (EOF) in the blubber of a killer whale (<i>Orcinus orca</i>) from Greenland suggests that some fluorinated substances preferentially bioaccumulate in storage lipids. To further investigate this, the present work examined blubber from 4 killer whales (3 from Greenland, 1 from Sweden) via gas chromatography-atmospheric pressure chemical ionization-ion mobility mass spectrometry. Using collision cross sections, we prioritized features suspected to be highly fluorinated and then selected 5 for manual annotation. Custom synthesized standards confirmed 10:2 and 12:2 fluorotelomer methylsulfone, 10:2 and 12:2 fluorotelomer chloromethylsulfone, and 6:2 bisfluorotelomer sulfone in all blubber samples from Greenland at concentrations ranging from &lt;0.4 to 72.5 ng/g, explaining 34–75% of blubber EOF, but none in the Swedish sample. None of these substances were observable in liver, suggesting preferential accumulation in storage lipids. To the best of our knowledge, this is the first report of neutral fluorotelomer sulfones in wildlife and the first identification of lipophilic, highly fluorinated PFAS.</p>","PeriodicalId":37,"journal":{"name":"Environmental Science & Technology Letters Environ.","volume":"12 9","pages":"1218–1224"},"PeriodicalIF":8.8,"publicationDate":"2025-08-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acs.estlett.5c00516","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145009650","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Experimental Determination of pKa for 10 PFAS, Mono-, Di-, and Trifluoroacetic Acid by 19F-NMR 用19F-NMR实验测定10种PFAS、单、二、三氟乙酸中的pKa
IF 8.8 2区 环境科学与生态学
Environmental Science & Technology Letters Environ. Pub Date : 2025-08-12 DOI: 10.1021/acs.estlett.5c00688
Damalka Balasuryia, Aina Queral-Beltran, Tristan Vick, Scott Simpson, Silvia Lacorte, Diana S. Aga and Alexander C. Hoepker*, 
{"title":"Experimental Determination of pKa for 10 PFAS, Mono-, Di-, and Trifluoroacetic Acid by 19F-NMR","authors":"Damalka Balasuryia,&nbsp;Aina Queral-Beltran,&nbsp;Tristan Vick,&nbsp;Scott Simpson,&nbsp;Silvia Lacorte,&nbsp;Diana S. Aga and Alexander C. Hoepker*,&nbsp;","doi":"10.1021/acs.estlett.5c00688","DOIUrl":"https://doi.org/10.1021/acs.estlett.5c00688","url":null,"abstract":"<p >Accurate p<i>K</i><sub>a</sub> values of per- and polyfluoroalkyl substances (PFAS) are urgently needed to improve predictions of their environmental fate, bioaccumulation, and removal, yet reliable experimental data remain scarce. Here, we determined the p<i>K</i><sub>a</sub> values of 10 PFAS and three short-chain fluorinated acids (MFA: 2.58 ± 0.03; DFA: 1.22 ± 0.03, TFA: 0.03 ± 0.08) using <sup>19</sup>F and <sup>1</sup>H NMR-based chemical shift perturbation. Results were compared to prior experimental values, OPERA predictions (CompTox), and our COSMO-RS calculations. Measured p<i>K</i><sub>a</sub> values include PFPrA (−0.18 to −0.54), PFOA (−0.27 ± 0.18), PFBS and PFOS (&lt; −1.85), 6:2 FTS (&lt;0.0), GenX (−0.20 ± 0.09), NFDHA (−0.32 ± 0.18), PFMPA (−0.26 ± 0.13), and 6:2 FTUCA (2.59 ± 0.11). Across C2, C3, and C8 homologues, PFCAs exhibit p<i>K</i><sub>a</sub> values of approximately −0.2 to −0.3. Telomerization markedly reduces acidity: 5:3 FTCA (p<i>K</i><sub>a</sub> = 4.05 ± 0.04) is &gt;10<sup>4</sup>-fold less acidic than PFOA, with COSMO-RS predicting similar effects from PFOS to 6:2 FTS. The dominant acidifying influence arises from CF<sub>2</sub> groups at C1 and C2 near COOH or SO<sub>3</sub>H. The unusually low p<i>K</i><sub>a</sub> values for TFA, PFOA, and GenX reflect our low-MeOH, sorption-resistant NMR method. COSMO-RS consistently outperformed OPERA, underscoring the need for experimental benchmarks to improve predictive models for emerging PFAS.</p>","PeriodicalId":37,"journal":{"name":"Environmental Science & Technology Letters Environ.","volume":"12 9","pages":"1238–1246"},"PeriodicalIF":8.8,"publicationDate":"2025-08-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acs.estlett.5c00688","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145009590","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
0
×
引用
GB/T 7714-2015
复制
MLA
复制
APA
复制
导出至
BibTeX EndNote RefMan NoteFirst NoteExpress
×
提示
您的信息不完整,为了账户安全,请先补充。
现在去补充
×
提示
您因"违规操作"
具体请查看互助需知
我知道了
×
提示
确定
请完成安全验证×
相关产品
×
本文献相关产品
联系我们:info@booksci.cn Book学术提供免费学术资源搜索服务,方便国内外学者检索中英文文献。致力于提供最便捷和优质的服务体验。 Copyright © 2023 布克学术 All rights reserved.
京ICP备2023020795号-1
ghs 京公网安备 11010802042870号
Book学术文献互助
Book学术文献互助群
群 号:604180095
Book学术官方微信