Wenlei Qin, Zhechao Hua, Kaiheng Guo and Jingyun Fang*,
{"title":"Thermodynamic and Kinetic Insights into Single Electron Transfer Pathway of Reactive Halogen Species: Is the Reduction Potential a Reliable Indicator for Radical Reactivity?","authors":"Wenlei Qin, Zhechao Hua, Kaiheng Guo and Jingyun Fang*, ","doi":"10.1021/acs.estlett.5c0047210.1021/acs.estlett.5c00472","DOIUrl":"https://doi.org/10.1021/acs.estlett.5c00472https://doi.org/10.1021/acs.estlett.5c00472","url":null,"abstract":"<p >Single electron transfer (SET) is the most important reaction mechanism of reactive halogen species (RHS) (e.g., Cl<sup>•</sup>, Cl<sub>2</sub><sup>•–</sup>, Br<sup>•</sup>, and Br<sub>2</sub><sup>•–</sup>) with aromatic contaminants. However, the key parameters governing the reactivity of RHS via the SET pathway remain unclear. This study comprehensively investigated the SET pathway of the RHS with 51 aromatic contaminants by quantum-chemical calculations. The calculated free energy changes of the SET pathway (Δ<i>G</i><sub>aq,SET</sub><sup>R</sup>) followed the order Cl<sup>•</sup> < Cl<sub>2</sub><sup>•–</sup> < Br<sup>•</sup> < Br<sub>2</sub><sup>•–</sup>, which was consistent with the order of their reduction potentials. However, the free energy of activation of the SET pathway (Δ<i>G</i><sub>aq,SET</sub><sup>⧧</sup>) followed a different order of Cl<sup>•</sup> < Br<sup>•</sup> < Cl<sub>2</sub><sup>•–</sup> < Br<sub>2</sub><sup>•–</sup>, which agreed with the order of their rate constants. This inconsistent trend between Δ<i>G</i><sub>aq,SET</sub><sup>R</sup> and Δ<i>G</i><sub>aq,SET</sub><sup>⧧</sup> for RHS reactions was attributed to the difference in reorganization energy, which is essentially related to the vertical electron affinity and radius of RHS. Therefore, the rate constants of SET reactions of RHS depend not only on their reduction potential but also on their vertical electron affinity and radius. These findings unravel the key factors determining the reactivity of RHS via the SET pathway and have profound implications for understanding other SET processes in water.</p>","PeriodicalId":37,"journal":{"name":"Environmental Science & Technology Letters Environ.","volume":"12 6","pages":"761–767 761–767"},"PeriodicalIF":8.9,"publicationDate":"2025-05-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144238352","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}
Yucheng Zhu, Hao Li, Junjie Wei, Hao Ding, Dongmei Cai, Xuan Zou, Guochen Wang, Qiongzhen Wang, Zhijian Ding, Ziwei Liu, Jia Chen, Long Yun, Congrui Deng and Kan Huang*,
{"title":"Marine Modulation of the Formation Pathways and Sources of Organosulfates over the Coastal South China Sea","authors":"Yucheng Zhu, Hao Li, Junjie Wei, Hao Ding, Dongmei Cai, Xuan Zou, Guochen Wang, Qiongzhen Wang, Zhijian Ding, Ziwei Liu, Jia Chen, Long Yun, Congrui Deng and Kan Huang*, ","doi":"10.1021/acs.estlett.5c0040610.1021/acs.estlett.5c00406","DOIUrl":"https://doi.org/10.1021/acs.estlett.5c00406https://doi.org/10.1021/acs.estlett.5c00406","url":null,"abstract":"<p >Organosulfates (OSs) constitute a considerable part of airborne sulfur-containing organic aerosols, influencing aerosol physicochemical properties, biogeochemical cycles, and climate. This study investigated the compositions, formation pathways, and sources of OSs at a coastal site of the South China Sea in summer. Thirty-three OS species were quantified by using an UHPLC-Orbitrap MS and were assessed under marine and terrestrial air mass origins. iOSs (isoprene-derived OSs) ranked the highest, followed by C2/C3 OSs (OSs with two or three carbon atoms). The formation of iOSs was influenced by aerosol pH and their major precursor (isoprene), with photochemical processes playing a significant role in terrestrial transport. Different from urban conditions, sea breezes favored the formation of 2-MAS (C<sub>4</sub>H<sub>7</sub>O<sub>7</sub>S<sup>–</sup>) over 2-MTS (C<sub>5</sub>H<sub>11</sub>O<sub>7</sub>S<sup>–</sup>) even under low NO<sub><i>x</i></sub> levels, mainly attributed to the high temperature and dominance of aqueous oxidation. Compared to terrestrial transport, the formation of C2/C3 OSs was more favored than that of iOSs under the influence of sea breezes. Marine biogenic emission was quantified as an important source of C2/C3 OSs. This study enhances our understanding of the influence of both terrestrial and marine factors on the formation pathways of atmospheric OSs and emphasizes the significant contribution of marine biogenic sources to OSs.</p>","PeriodicalId":37,"journal":{"name":"Environmental Science & Technology Letters Environ.","volume":"12 6","pages":"739–746 739–746"},"PeriodicalIF":8.9,"publicationDate":"2025-05-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144238734","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}
Felix R. Harris, Mark D. Jankowski, Daniel L. Villeneuve and Joshua A. Harrill*,
{"title":"Phenotypic Profiling of 6PPD, 6PPD-Quinone, and Structurally Diverse Antiozonants in RTgill-W1 Cells Using the Cell Painting Assay","authors":"Felix R. Harris, Mark D. Jankowski, Daniel L. Villeneuve and Joshua A. Harrill*, ","doi":"10.1021/acs.estlett.5c0032710.1021/acs.estlett.5c00327","DOIUrl":"https://doi.org/10.1021/acs.estlett.5c00327https://doi.org/10.1021/acs.estlett.5c00327","url":null,"abstract":"<p >6PPD-quinone, a degradation product of the rubber antiozonant 6PPD that is frequently added to tires, has previously been identified as a causative agent of urban runoff mortality syndrome in salmonids. Previous high-throughput phenotypic profiling (HTPP) studies using the Cell Painting assay in the RTgill-W1 rainbow trout cell line have demonstrated that 6PPD-quinone toxicity occurs at much lower concentrations than the 6PPD parent molecule, which is consistent with available <i>in vivo</i> toxicity data in rainbow trout. Current research efforts include identifying alternative antiozonant compounds to potentially replace 6PPD in tire manufacturing. To fill bioactivity data gaps for potential 6PPD alternatives, 18 compounds including other substituted <i>p</i>-phenylenediamines (PPD) and PPD-quinones were assayed using HTPP in RTgill-W1 cells. 7PPD-quinone and 77PD-quinone produced changes in cellular phenotype similar to those of 6PPD-quinone at comparable concentrations. IPPD-quinone produced changes in cellular phenotype at higher concentrations than 6PPD-quinone, with a phenotypic profile that was most similar to its parent molecule IPPD. These findings suggest that 7PPD-quinone and 77PD-quinone may exhibit similar effects in rainbow trout and potentially other 6PPD-quinone sensitive salmonids. In contrast, IPPD may be less toxic to salmonids than 6PPD, given the relative lack of bioactivity of IPPD-quinone compared to 6PPD-quinone.</p>","PeriodicalId":37,"journal":{"name":"Environmental Science & Technology Letters Environ.","volume":"12 6","pages":"695–701 695–701"},"PeriodicalIF":8.9,"publicationDate":"2025-05-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144238928","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}
Charles Gan, Melissa Pitton, Jolinda de Korne-Elenbaas, Ludovico Cobuccio, Alessandro Cassini, Christoph Ort and Timothy R. Julian*,
{"title":"Retrospective Wastewater Tracking of Measles Outbreak in Western Switzerland in Winter 2024","authors":"Charles Gan, Melissa Pitton, Jolinda de Korne-Elenbaas, Ludovico Cobuccio, Alessandro Cassini, Christoph Ort and Timothy R. Julian*, ","doi":"10.1021/acs.estlett.5c0024410.1021/acs.estlett.5c00244","DOIUrl":"https://doi.org/10.1021/acs.estlett.5c00244https://doi.org/10.1021/acs.estlett.5c00244","url":null,"abstract":"<p >Measles outbreaks remain a significant public health challenge, despite high vaccination coverage in many regions. Wastewater-based surveillance (WBS) offers a noninvasive and community-level approach to monitoring the circulation of pathogens, including the measles virus. Here, we retrospectively applied a duplex digital PCR assay to distinguish between wild-type and vaccine strains of the measles virus in wastewater samples available from an existing national WBS program. Samples originated from the wastewater treatment plant serving the Lausanne city catchment area, where an outbreak occurred before spreading to the broader Canton Vaud region. Despite high vaccination rates, viral loads of the measles wild type were detected during the first transmission event involving 21 cases identified within a week. However, viral loads were no longer detectable after the initial 21 cases, despite an additional 30 cases reported in the following 3 weeks, possibly due to lower incidence rate or location outside the catchment. Measles vaccine strain was not detected during the outbreak. Our results demonstrate the complementarity of WBS with clinical surveillance and suggest its potential as an early warning system for measles and other vaccine-preventable diseases. Further improvements in the assay sensitivity and integration with epidemiological data could enhance the utility of WBS for outbreak detection and control.</p>","PeriodicalId":37,"journal":{"name":"Environmental Science & Technology Letters Environ.","volume":"12 6","pages":"689–694 689–694"},"PeriodicalIF":8.9,"publicationDate":"2025-05-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acs.estlett.5c00244","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144238504","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}
Charles Gan, Melissa Pitton, Jolinda de Korne-Elenbaas, Ludovico Cobuccio, Alessandro Cassini, Christoph Ort, Timothy R Julian
{"title":"Retrospective Wastewater Tracking of Measles Outbreak in Western Switzerland in Winter 2024.","authors":"Charles Gan, Melissa Pitton, Jolinda de Korne-Elenbaas, Ludovico Cobuccio, Alessandro Cassini, Christoph Ort, Timothy R Julian","doi":"10.1021/acs.estlett.5c00244","DOIUrl":"10.1021/acs.estlett.5c00244","url":null,"abstract":"<p><p>Measles outbreaks remain a significant public health challenge, despite high vaccination coverage in many regions. Wastewater-based surveillance (WBS) offers a noninvasive and community-level approach to monitoring the circulation of pathogens, including the measles virus. Here, we retrospectively applied a duplex digital PCR assay to distinguish between wild-type and vaccine strains of the measles virus in wastewater samples available from an existing national WBS program. Samples originated from the wastewater treatment plant serving the Lausanne city catchment area, where an outbreak occurred before spreading to the broader Canton Vaud region. Despite high vaccination rates, viral loads of the measles wild type were detected during the first transmission event involving 21 cases identified within a week. However, viral loads were no longer detectable after the initial 21 cases, despite an additional 30 cases reported in the following 3 weeks, possibly due to lower incidence rate or location outside the catchment. Measles vaccine strain was not detected during the outbreak. Our results demonstrate the complementarity of WBS with clinical surveillance and suggest its potential as an early warning system for measles and other vaccine-preventable diseases. Further improvements in the assay sensitivity and integration with epidemiological data could enhance the utility of WBS for outbreak detection and control.</p>","PeriodicalId":37,"journal":{"name":"Environmental Science & Technology Letters Environ.","volume":"12 6","pages":"689-694"},"PeriodicalIF":8.9,"publicationDate":"2025-05-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC12160055/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144300694","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}
Jian Liu, Jason Blake Cohen*, Ye Feng, Shuo Wang and Kai Qin,
{"title":"OMI-Derived Mass- and Number-Conserved Estimation of Black Carbon Emissions","authors":"Jian Liu, Jason Blake Cohen*, Ye Feng, Shuo Wang and Kai Qin, ","doi":"10.1021/acs.estlett.5c0034010.1021/acs.estlett.5c00340","DOIUrl":"https://doi.org/10.1021/acs.estlett.5c00340https://doi.org/10.1021/acs.estlett.5c00340","url":null,"abstract":"<p >Black carbon (BC) emission estimates remain highly uncertain, especially in regions impacted by biomass burning (BB) and rapid urban expansion, where emissions are temporally variable and often misrepresented in bottom-up inventories(<contrib-group><span>Liu, J.</span>; <span>Cohen, J. B.</span>; <span>He, Q.</span>; <span>Tiwari, P.</span>; <span>Qin, J.</span></contrib-group> Accounting for NO<sub>x</sub> Emissions from Biomass Burning and Urbanization Doubles Existing Inventories over South, Southeast and East Asia. <cite><i>Commun. Earth Environ.</i></cite> <span>2024</span>, <em>5</em> (1), 1−16. <contrib-group><span>Lu, L.</span>; <span>Cohen, J. B.</span>; <span>Qin, K.</span>; <span>Li, X.</span>; <span>He, Q.</span></contrib-group> Identifying Missing Sources and Reducing NO<sub>x</sub> Emissions Uncertainty over China Using Daily Satellite Data and a Mass-Conserving Method. <cite><i>Atmos. Chem. Phys.</i></cite> <span>2025</span>, <em>25</em> (4), 2291−2309. <contrib-group><span>Tiwari, P.</span>; <span>Cohen, J. B.</span>; <span>Lu, L.</span>; <span>Wang, S.</span>; <span>Li, X.</span>; <span>Guan, L.</span>; <span>Liu, Z.</span>; <span>Li, Z.</span>; <span>Qin, K.</span></contrib-group> Multi-platform observations and constraints reveal overlooked urban sources of black carbon in Xuzhou and Dhaka. <cite><i>Commun. Earth Environ.</i></cite> <span>2025</span>, <em>6</em> (1), 1−20.). This study introduces a novel top-down approach using the OMI-derived column densities of BC mass and number to estimate emissions via mass- and number-conservative methods. The analysis spans all of 2016 across South, Southeast, and East Asia, with particular focus on February to May─months marked by intensified BB and urban pollution events using an unbiased technique(<contrib-group><span>Hawkins, L. R.</span>; <span>Abatzoglu, J. T.</span>; <span>Li, S.</span>; <span>Rupp, D. E.</span></contrib-group> Anthropogenic Influence on Recent Severe Autumn Fire Weather in 414 the West Coast of the United States. <cite><i>Geophys. Res. Lett.</i></cite> <span>2022</span>, <em>49</em> (4), e2021GL095496. <contrib-group><span>Jain, P.</span></contrib-group>, Drivers and Impacts of the Record-Breaking 2023 Wildfire Season in Canada. <cite><i>Nat. Commun.</i></cite> <span>2024</span>, <em>15</em> (1), 6764.). Estimated total BC emissions are 205 (+55.0, −127) Gg and 247 (+50.0, −154) Gg for the mass- and number-conserved methods, respectively, exceeding FINN and EDGAR-HTAP inventory values by factors of 15.0 and 18.2, but of similar magnitude to regional average top-down studies (<contrib-group><span>Cohen, J. B.</span>; <span>Wang, C.</span></contrib-group> Estimating global black carbon emissions using a top-down Kalman Filter approach. <cite><i>J. Geophys. Res.: Atmos.</i></cite> <span>2014</span>, <em>119</em> (1), 307−323. <contrib-group><span>Chen, C.</span></contrib-group>, Multi-angular polarimetric remote sensing to pinpoint global aerosol absorpt","PeriodicalId":37,"journal":{"name":"Environmental Science & Technology Letters Environ.","volume":"12 6","pages":"731–738 731–738"},"PeriodicalIF":8.9,"publicationDate":"2025-05-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144238772","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}