Environmental Science & Technology Letters Environ.最新文献_第5页

Quantitative Imaging of Polyfluoroalkyl Substances Based on the Reversal of Albumin Luminescence 基于白蛋白发光反转的多氟烷基物质定量成像

IF 7.3 2区环境科学与生态学

Environmental Science & Technology Letters Environ. Pub Date : 2026-08-11 Epub Date: 2026-07-31 DOI: 10.1021/acs.estlett.6c00408

Sung-Bae Kim, Sachi Taniyasu, Tadaomi Furuta, Nobuo Kitada, Suresh Thangudu, Arutselvan Natarajan, Shojiro A. Maki, Ramasamy Paulmurugan

{"title":"Quantitative Imaging of Polyfluoroalkyl Substances Based on the Reversal of Albumin Luminescence","authors":"Sung-Bae Kim, Sachi Taniyasu, Tadaomi Furuta, Nobuo Kitada, Suresh Thangudu, Arutselvan Natarajan, Shojiro A. Maki, Ramasamy Paulmurugan","doi":"10.1021/acs.estlett.6c00408","DOIUrl":"https://doi.org/10.1021/acs.estlett.6c00408","url":null,"abstract":"Per- and polyfluoroalkyl substances (PFASs) are human-madeenvironmentalcontaminants of global concern due to their extreme persistence andpotential adverse health effects, and elucidating their physiologicalimpacts remains a critical challenge. In this study, we present amolecular imaging platform that enables quantitative visualizationof PFAS effects in vivo and in vitro by indexing the reversal of albumin luminescence mediated by speciallydesigned coelenterazine (CTZ) analogues as optical indicators. Wesynthesized a list of CTZ analogues to facilitate luminescence uponbinding with specific albumins; this signal is efficiently suppressedby PFAS compounds. We found that perfluorooctanoic acid (PFOA) andperfluorooctanesulfonic acid (PFOS) dose dependently suppressed bovineserum albumin luminescence, a feature consistent across multiple mammalianalbumins, including humans. Further in vivo imagingrevealed rapid absorption of PFOS into the liver of living mice anda marked 41% reduction in hepatic luminescence, suggesting that acuteexposure suppresses the normal liver activity. This study representsthe first albumin-based molecular imaging platform for assaying thepotential physiological impacts of PFASs in vivo and in vitro, offering a practical and adaptable tool for environmentalmonitoring and toxicological evaluation.","PeriodicalId":37,"journal":{"name":"Environmental Science & Technology Letters Environ.","volume":"13 8","pages":"1049–1055"},"PeriodicalIF":7.3,"publicationDate":"2026-08-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148709916","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

Distance-Dependent Transport of Tire and Road Wear Particles along the Road-to-Indoor Gradient and Implications for Human Exposure 轮胎和道路磨损颗粒沿道路到室内梯度的距离依赖运输及其对人类暴露的影响

IF 7.3 2区环境科学与生态学

Environmental Science & Technology Letters Environ. Pub Date : 2026-08-11 Epub Date: 2026-07-30 DOI: 10.1021/acs.estlett.6c00413

Yutong Sui, Yifan Ren, Chen Qu, Yu Chen, Yanjun Zhao, Wenhui Li, Chuandong Wu, Jiemin Liu

{"title":"Distance-Dependent Transport of Tire and Road Wear Particles along the Road-to-Indoor Gradient and Implications for Human Exposure","authors":"Yutong Sui, Yifan Ren, Chen Qu, Yu Chen, Yanjun Zhao, Wenhui Li, Chuandong Wu, Jiemin Liu","doi":"10.1021/acs.estlett.6c00413","DOIUrl":"https://doi.org/10.1021/acs.estlett.6c00413","url":null,"abstract":"Tire and road wear particles (TRWPs)are ubiquitous inurban environmentsand represent a potential pathway for human exposure to microplastics,yet knowledge of their transport across multimedia and the associatedexposure implications remains scarce. Here, we investigate the road-to-indoortransport of TRWPs and evaluate human exposure in road-adjacent andindoor scenarios using a multicompartment nationwide data set. Lateraland vertical transport analysis showed clear attenuation with increasingroad-to-building distance and sampling height, following the relationships y = 1.62x–0.384 and y = 1.16e–0.023x, respectively.Particle size played a dominant role in transport, with finer particlesshowing greater indoor penetration. In contrast, aspect ratio variedlittle among compartments and exerted limited influence. Wind speedfurther affected TRWP transport, showing a positive correlation withlateral transport (r = 0.398) but a negative correlationwith vertical transport (r = −0.512). Moreover,TRWPs contribute to daily intake in both outdoor and indoor environments,with dust ingestion being the predominant pathway. Notably, indoorexposure exceeded outdoor exposure, with median estimated daily intakesof 12 300 and 928 ng (kg of body weight)−1 day–1 for children and adults, respectively. Thisstudy provides new insights into the transport patterns of TRWPs andhighlights their substantial contribution to human exposure in road-to-indoorenvironments.","PeriodicalId":37,"journal":{"name":"Environmental Science & Technology Letters Environ.","volume":"13 8","pages":"1164–1169"},"PeriodicalIF":7.3,"publicationDate":"2026-08-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148709928","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

Service Line Characterization via Handheld Lead K-Shell X-ray Fluorescence 通过手持式铅k壳x射线荧光表征服务线

IF 7.3 2区环境科学与生态学

Environmental Science & Technology Letters Environ. Pub Date : 2026-08-11 Epub Date: 2026-07-09 DOI: 10.1021/acs.estlett.6c00528

Michael K. DeSantis, Chantaly Villalona, Jennifer Tully

{"title":"Service Line Characterization via Handheld Lead K-Shell X-ray Fluorescence","authors":"Michael K. DeSantis, Chantaly Villalona, Jennifer Tully","doi":"10.1021/acs.estlett.6c00528","DOIUrl":"https://doi.org/10.1021/acs.estlett.6c00528","url":null,"abstract":"Lead-lined galvanized iron pipe (LLGIP), installed acrossthe USAduring the early 1900s, often goes underreported because of visualexterior similarities and physical material characteristics to galvanizediron pipes (GIPs). However, their interior lead lining interacts withdrinking water like traditional lead service lines and will be treatedas such in accordance with the USEPA’s Lead and Copper RuleImprovements. Handheld X-ray fluorescence (hhXRF), widely used forelemental analyses of various matrices, is a potential service lineidentification tool, but it has not yet been comprehensively testedin a controlled setting for this application. This study evaluatedthe applicability of 57Co K-shell hhXRF as a method foridentifying service line materials. A total of 88 exhumed field pipeswere gathered and analyzed. Lead results revealed a significantlylower average lead count of 282 (σ 222) cps for GIPs comparedto an average of 8,696 (σ 5,861) cps for LLGIPs. The study resultsdemonstrated under laboratory conditions the hhXRF’s abilityto 100% successfully differentiate between GIPs and LLGIPs throughexterior analysis, a distinction previously only available by physicalextraction of the pipe or water sampling. hhXRF did not consistentlydistinguish LLGIP from brass; thus, existing physical methods arestill needed for these materials.","PeriodicalId":37,"journal":{"name":"Environmental Science & Technology Letters Environ.","volume":"13 8","pages":"1071–1076"},"PeriodicalIF":7.3,"publicationDate":"2026-08-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148703592","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

Emissions of Volatile Methyl Siloxanes (VMS) from Vehicles 车辆挥发性甲基硅氧烷（VMS）排放

IF 7.3 2区环境科学与生态学

Environmental Science & Technology Letters Environ. Pub Date : 2026-08-11 Epub Date: 2026-07-11 DOI: 10.1021/acs.estlett.6c00590

Yanfang Chen, Yuantao Wang, Siyao Yue, Michael Bauer, Damianos Pavlidis, Carolina Molina, Georgia A. Argyropoulou, Andreas Aktypis, Christos Kaltsonoudis, Philippe Wili, Pierre Comte, Danilo Engelmann, Athanasios Nenes, Christian George, Imad El Haddad, Jay G. Slowik, Spyros N. Pandis, Andre S. H. Prevot, David M. Bell

{"title":"Emissions of Volatile Methyl Siloxanes (VMS) from Vehicles","authors":"Yanfang Chen, Yuantao Wang, Siyao Yue, Michael Bauer, Damianos Pavlidis, Carolina Molina, Georgia A. Argyropoulou, Andreas Aktypis, Christos Kaltsonoudis, Philippe Wili, Pierre Comte, Danilo Engelmann, Athanasios Nenes, Christian George, Imad El Haddad, Jay G. Slowik, Spyros N. Pandis, Andre S. H. Prevot, David M. Bell","doi":"10.1021/acs.estlett.6c00590","DOIUrl":"https://doi.org/10.1021/acs.estlett.6c00590","url":null,"abstract":"Volatile methyl siloxanes (VMS) are anthropogenic compoundswidelyused in personal care products and industrial applications and arefrequently detected at elevated concentrations in urban air. However,their sources in urban areas remain poorly constrained. Here, we usechassis dynamometer experiments to quantify gas-phase VMS emissionsfrom a range of on-road vehicles, including light-duty gasoline anddiesel vehicles. Hexamethylcyclotrisiloxane (D3) dominatedthe emitted VMS, over octamethylcyclotetrasiloxane (D4),and decamethylcyclopentasiloxane (D5). VMS emissions increasedwith driving speed and were substantially higher from gasoline thanfrom diesel vehicles. Comparison with tunnel measurements showingelevated ambient VMS concentrations supports a significant contributionfrom traffic-related sources, including tailpipe and potentially nontailpipeemissions. These results identify vehicular emissions as a previouslyunderrecognized source of VMS near highways, and provide new constraintsfor their atmospheric budget and source apportionment.","PeriodicalId":37,"journal":{"name":"Environmental Science & Technology Letters Environ.","volume":"13 8","pages":"1145–1150"},"PeriodicalIF":7.3,"publicationDate":"2026-08-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148703597","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

Trifluoroacetic Acid (TFA) Exceeds All Other Extractable Organofluorine in Drinking Water from Eastern Massachusetts, United States 美国马萨诸塞州东部饮用水中的三氟乙酸（TFA）超过所有其他可提取有机氟

IF 7.3 2区环境科学与生态学

Environmental Science & Technology Letters Environ. Pub Date : 2026-08-11 Epub Date: 2026-07-09 DOI: 10.1021/acs.estlett.6c00404

Jahred M. Liddie, Euna Kim, Faiz Haque, Anton Roche, Ethan J. Sontarp, Elsie M. Sunderland

{"title":"Trifluoroacetic Acid (TFA) Exceeds All Other Extractable Organofluorine in Drinking Water from Eastern Massachusetts, United States","authors":"Jahred M. Liddie, Euna Kim, Faiz Haque, Anton Roche, Ethan J. Sontarp, Elsie M. Sunderland","doi":"10.1021/acs.estlett.6c00404","DOIUrl":"https://doi.org/10.1021/acs.estlett.6c00404","url":null,"abstract":"Per- and polyfluoroalkyl substances (PFAS) are presentin drinkingwater consumed by ∼200 million United States (US) residents,but many are not detected by routine monitoring methods. Here, weaimed to better characterize the organofluorine mass budget in USdrinking water samples from 19 sites in eastern Massachusetts. Extractableorganofluorine (EOF) was detected at 16/17 sites served by communitywater systems (CWS) using conventional treatment techniques (coagulation,flocculation, clarification, and filtration). At these sites, a suiteof 37 targeted PFAS accounted for 6–68% of the EOF and suspectscreening identified fluorinated agrochemicals in almost all samples.High EOF concentrations in untreated source waters for two CWS thatused granular activated carbon (GAC) and ion-exchange (IX) treatment,were reduced below detection in finished drinking water samples. OurEOF measurements were not selective for trifluoroacetic acid (TFA),so we measured concentrations in triplicate samples at one conventionaltreatment site and from the IX and GAC sites. At these sites, TFAconcentrations were higher than those of EOF and were unaffected bythe treatment type. Results of this pilot study show GAC and IX treatmentremoved virtually all organofluorine in drinking water other thanTFA.","PeriodicalId":37,"journal":{"name":"Environmental Science & Technology Letters Environ.","volume":"13 8","pages":"1157–1163"},"PeriodicalIF":7.3,"publicationDate":"2026-08-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148703593","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

Upcycling Arsenic Trioxide Waste to Form Arsenic(0) Metal: A New Approach to Manage Legacy Arsenic Pollution 升级回收三氧化二砷废物形成砷(0)金属：治理遗留砷污染的新途径

IF 7.3 2区环境科学与生态学

Environmental Science & Technology Letters Environ. Pub Date : 2026-08-11 Epub Date: 2026-07-11 DOI: 10.1021/acs.estlett.6c00409

Kaifeng Wang, Tamara R. Etmannski, Case M. van Genuchten

{"title":"Upcycling Arsenic Trioxide Waste to Form Arsenic(0) Metal: A New Approach to Manage Legacy Arsenic Pollution","authors":"Kaifeng Wang, Tamara R. Etmannski, Case M. van Genuchten","doi":"10.1021/acs.estlett.6c00409","DOIUrl":"https://doi.org/10.1021/acs.estlett.6c00409","url":null,"abstract":"Upcycling solid arsenic (As)-bearing waste to producemetallicAs(0), a critical raw material (CRM) with growing industrial applications,represents a new approach to manage legacy As pollution that can alsobenefit local communities affected by carcinogenic waste. In thiswork, we demonstrate metallic As(0) forms readily from solid As2O3-bearing waste from Giant Mine (Yellowknife,Canada), one of the largest legacy As-rich waste sites in the world,via an upcycling process consisting of aqueous dissolution and subsequentreductive As(0) precipitation. We found that up to >99% of thesolid-phaseAs in the ATRW dissolved in both pure water and 0.1 M NaOH, thoughNaOH increased As dissolution kinetics and enhanced the dissolutionof antimony (Sb) contained in the ATRW. Dosing thiourea dioxide (TDO)reductively precipitated up to >99% of the aqueous As, yieldingpoorlycrystalline or amorphous As(0) with a purity >99% As in optimalconditions.However, coprecipitation of aqueous Sb lowered As(0) purity, indicatinga trade-off in the use of NaOH as the dissolution medium. This proof-of-conceptstudy sets the stage for future research to upscale the chemical upcyclingprocess and evaluate the long-term environmental benefits and risksof this approach.","PeriodicalId":37,"journal":{"name":"Environmental Science & Technology Letters Environ.","volume":"13 8","pages":"1198–1203"},"PeriodicalIF":7.3,"publicationDate":"2026-08-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148703594","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

Scanning Electron Microscopy as a Potential Tool for Distinguishing Charcoal from Dark, Oxidized Biomass 扫描电子显微镜作为区分木炭和深色氧化生物质的潜在工具

IF 7.3 2区环境科学与生态学

Environmental Science & Technology Letters Environ. Pub Date : 2026-08-11 Epub Date: 2026-07-17 DOI: 10.1021/acs.estlett.6c00241

João Vitor dos Santos, Aleksandar I. Goranov, Lais Gomes Fregolente, João Marcos de Lima-Faria, Diego Stéfani Teodoro Martinez, Patrick G. Hatcher

{"title":"Scanning Electron Microscopy as a Potential Tool for Distinguishing Charcoal from Dark, Oxidized Biomass","authors":"João Vitor dos Santos, Aleksandar I. Goranov, Lais Gomes Fregolente, João Marcos de Lima-Faria, Diego Stéfani Teodoro Martinez, Patrick G. Hatcher","doi":"10.1021/acs.estlett.6c00241","DOIUrl":"https://doi.org/10.1021/acs.estlett.6c00241","url":null,"abstract":"Condensed aromatic carbon (ConAC) is widely used as aproxy fororganic materials derived from biomass burning. However, recent evidenceshows that ConAC can be also formed through nonpyrogenic oxidativeprocesses. This study presents a proof-of-concept investigation usingscanning electron microscopy (SEM) to distinguish charcoal from dark,ConAC-rich materials produced by ambient oxidation of biomass. Pinewood exposed to long-term iron-mediated oxidation was compared withunaltered wood and a controlled laboratory-generated charcoal reference.Conventional geochemical analytical methods, including benzenepoly(carboxylicacid) (BPCA) analysis, Fourier transform–ion cyclotron resonance–massspectrometry (FT-ICR-MS), solid-state 13C nuclear magneticresonance (NMR) spectroscopy, and elemental analysis, confirmed substantialnonpyrogenic formation of ConAC in the oxidized wood. SEM imagingrevealed that the oxidized biomass retained the native wood cellularfeatures, including secondary wall layering and compound middle lamella,closely resembling unaltered wood. In contrast, the charcoal referenceexhibited collapsed and homogenized cellular microstructures. Theseclear morphological differences between the different formation pathwayssuggest that microstructural preservation may serve as a useful diagnosticindicator for differentiating pyrogenic and nonpyrogenic charcoal-likematerials. Thus, incorporating SEM-based screening alongside geochemicalanalyses can potentially improve source attribution of ConAC and refineinterpretations of fire history and refractory carbon cycling in environmentalsystems.","PeriodicalId":37,"journal":{"name":"Environmental Science & Technology Letters Environ.","volume":"13 8","pages":"1092–1100"},"PeriodicalIF":7.3,"publicationDate":"2026-08-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148709886","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

Ammonia Synergistic Effects and Stability Evolution in Sulfuric Acid-Dimethylamine Clusters up to 10 Molecules 10分子以下硫酸-二甲胺团簇中氨的协同效应及其稳定性演化

IF 7.3 2区环境科学与生态学

Environmental Science & Technology Letters Environ. Pub Date : 2026-08-11 Epub Date: 2026-07-31 DOI: 10.1021/acs.estlett.6c00614

Yuze Han, Zhengning Xu, Jian Gao, Qingye Liu, Zhibin Wang

引用次数: 0

Relevance of Sustainable and Green-Synthesized Biogenic Iron Oxide Nanoparticles for Remediation of Emerging Contaminants from Water Ecosystems and Their Associated Health Concerns 可持续和绿色合成的生物氧化铁纳米颗粒对水生态系统中新出现的污染物及其相关健康问题的修复的相关性

IF 7.3 2区环境科学与生态学

Environmental Science & Technology Letters Environ. Pub Date : 2026-08-11 Epub Date: 2026-07-17 DOI: 10.1021/acs.estlett.6c00068

Gagandeep Singh, Rakesh Kumar, Neelam Thakur, Umesh Kumar, Prosun Bhattacharya

{"title":"Relevance of Sustainable and Green-Synthesized Biogenic Iron Oxide Nanoparticles for Remediation of Emerging Contaminants from Water Ecosystems and Their Associated Health Concerns","authors":"Gagandeep Singh, Rakesh Kumar, Neelam Thakur, Umesh Kumar, Prosun Bhattacharya","doi":"10.1021/acs.estlett.6c00068","DOIUrl":"https://doi.org/10.1021/acs.estlett.6c00068","url":null,"abstract":"Groundwater pollution by emerging contaminants (ECs),includingpharmaceuticals, per- and polyfluoroalkyl substances (PFAS), heavymetals, and disinfection byproducts, poses severe environmental andpublic health hazards. Conventional treatment approaches are unableto eliminate ECs, prompting the development of sustainable alternativesfor eliminating ECs. This review provides insights into the synthesisof iron oxide nanoparticles (IONPs) using environmentally friendlymethods, including systems based on bacteria, fungi, algae, plants,and biowaste. Biogenic IONPs are highly effective at removing ECs,including PFAS, certain medications, and organic pollutants. Theirunusual physicochemical characteristics, high surface area, magneticseparation capability, and tunable reactivity make them promisingcandidates for groundwater cleanup. Future studies should focus onexpanding the application of IONPs across a broader range of ECs,refining synthesis methods, and improving functionalization to enabletargeted pollutant removal. Though knowledge gaps exist regardingtheir efficiency against some contaminants, e.g., persistent pesticides,nitrosamines, microplastics, and complex pharmaceutical metabolites,for which no effective biogenic IONPs are currently available, biogenicIONPs have shown great potential for removing several ECs. BiogenicIONPs are a long-lasting and effective way to mitigate health risksand groundwater contamination provided that they are continually improved.","PeriodicalId":37,"journal":{"name":"Environmental Science & Technology Letters Environ.","volume":"13 8","pages":"1029–1048"},"PeriodicalIF":7.3,"publicationDate":"2026-08-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148703624","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

Size-Dependent Reaction Pathways in Multiphase SO2 Oxidation Chemistry 多相SO2氧化化学中粒径依赖的反应途径

IF 7.3 2区环境科学与生态学

Environmental Science & Technology Letters Environ. Pub Date : 2026-08-11 Epub Date: 2026-07-07 DOI: 10.1021/acs.estlett.6c00512

Kedong Gong, Adriane Tam, V. Faye McNeill, Vicki H. Grassian

{"title":"Size-Dependent Reaction Pathways in Multiphase SO2 Oxidation Chemistry","authors":"Kedong Gong, Adriane Tam, V. Faye McNeill, Vicki H. Grassian","doi":"10.1021/acs.estlett.6c00512","DOIUrl":"https://doi.org/10.1021/acs.estlett.6c00512","url":null,"abstract":"The paradigm foratmospheric multiphase SO2 chemistry,traditionally based on bulk aqueous-phase studies, involves a multistepprocess of SO2 uptake followed by oxidation. Here, we decouplethese steps at the single-droplet level by comparing SO2 uptake and reported dissolved S(IV)(aq) oxidation in aqueous microdropletsof varying sizes. Our results reveal that SO2 uptake intomicrodroplets to form S(IV)(aq) is suppressed as the droplet radius(r) decreases, in contrast to our previous findingthat S(IV)(aq) oxidation is enhanced at smaller radii. Fitting theseopposing size-dependent processes shows that SO2 uptakeis 1–2 orders of magnitude slower than S(IV)(aq) oxidationfor typical atmospheric aerosols (r ≲ 5 μm).Thus, larger cloud and fog microdroplets follow the conventional bulk-phasepathway while smaller aqueous aerosols become uptake-limited and favordirect oxidation at the surface. Mn(II)-catalyzed SO2 oxidationin Na2SO3 microdroplets with contrasting radii(r = 5.9 and 94.0 μm) further supports thissize-dependent mechanistic transition. Overall, by distinguishingSO2 uptake from subsequent S(IV)(aq) oxidation, we showthat size can modulate the rate-limiting step, leading to differentmultiphase SO2 oxidation mechanisms. This step-specificperspective highlights the critical and multiple roles of the air–waterinterface and emphasizes how different size dependencies in individualsteps within a multistep mechanism can further our understanding ofatmospheric multiphase chemistry.","PeriodicalId":37,"journal":{"name":"Environmental Science & Technology Letters Environ.","volume":"13 8","pages":"1132–1138"},"PeriodicalIF":7.3,"publicationDate":"2026-08-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148703609","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