{"title":"New insight into the spatiotemporal distribution and ecological risk assessment of endocrine-disrupting chemicals in the Minjiang and Tuojiang rivers: perspective of watershed landscape patterns†","authors":"Weike Zhao, Peilin Li and Bo Yang","doi":"10.1039/D4EM00052H","DOIUrl":"10.1039/D4EM00052H","url":null,"abstract":"<p >This study evaluated the pollution characteristics, spatiotemporal distribution, and ecological risks of eight endocrine-disrupting chemicals (EDCs) in the Minjiang and Tuojiang rivers. Utilizing 3S technology (ArcGIS, remote sensing, GPS) and Fragstats, the research calculated eight landscape pattern indices related to land use types along the Minjiang river and established correlations between landscape factors and EDC distribution through stepwise multiple regression. The results indicated that bisphenol A (BPA) and nonylphenol (NP) were the most concerning EDCs, with detection frequencies of 97–100% and peak concentrations up to 63.35 ng L<small><sup>−1</sup></small>, primarily located in the middle and lower reaches of the Minjiang river and the upper reaches of the Tuojiang river. There was a significant correlation between the spatial distribution of pollutants and landscape patterns, where increased fragmentation, a higher number of patches, and complex patch shapes within a 10-kilometer buffer zone were associated with elevated levels of river pollution. By integrating four classical mathematical models to fit curves for acute and chronic toxicity data of BPA and NP, the findings suggested that BPA posed a higher ecological risk. This interdisciplinary research provided essential theoretical insights for investigating river pollution and its influencing factors, offering a new perspective on simultaneous river pollution control, urban functional zoning, and adjustment of watershed landscape spatial patterns from an urban planning standpoint.</p>","PeriodicalId":74,"journal":{"name":"Environmental Science: Processes & Impacts","volume":" 8","pages":" 1360-1372"},"PeriodicalIF":4.3,"publicationDate":"2024-07-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141490042","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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}
Zerong Guan, Xueqiong Weng, Ligang Zhang and Peiran Feng
{"title":"Association between polycyclic aromatic hydrocarbon exposure and cognitive performance in older adults: a cross-sectional study from NHANES 2011–2014†","authors":"Zerong Guan, Xueqiong Weng, Ligang Zhang and Peiran Feng","doi":"10.1039/D4EM00290C","DOIUrl":"10.1039/D4EM00290C","url":null,"abstract":"<p > <em>Background</em>: polycyclic aromatic hydrocarbons (PAHs) are classified as neurotoxins, but the relationship between exposure to PAHs and cognition in adults is unclear, and their non-linear and mixed exposure association hasn't been explored. <em>Objective</em>: to evaluate the non-linear and joint association between co-exposure to PAHs and multiple cognitive tests in U.S. older people. <em>Methods</em>: restricted cubic spline (RCS) and Bayesian kernel machine regression (BKMR) were conducted to evaluate the non-linear and mixed exposure association, based on the cross-sectional data from NHANES 2011–2014: 772 participants over 60 years old, 4 cognitive test scores, including the Immediate Recall Test (IRT), Delayed Recall Test (DRT), Animal Fluency Test (AFT), and Digit Symbol Substitution test (DSST), and 5 urinary PAH metabolites. <em>Results</em>: a V-shaped nonlinear relationship was found between 3-hydroxyfluorene (3-FLUO), 2-hydroxyfluorene (2-FLUO), and DRT. Negative trends between mixed PAH exposure and IRT, DRT, and DSST scores were observed. 2-FLUO contributed the most to the negative association of multiple PAHs with IRT and DRT scores and 2-hydroxynaphthalene (2-NAP) played the most important role in the decreasing relationship between mixed PAH exposure and DSST scores. <em>Conclusion</em>: our study suggested that PAH exposure in the U.S. elderly might be related to their poor performances in IRT, DRT and DSST. Further prospective studies are needed to validate the association.</p>","PeriodicalId":74,"journal":{"name":"Environmental Science: Processes & Impacts","volume":" 8","pages":" 1348-1359"},"PeriodicalIF":4.3,"publicationDate":"2024-07-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141490041","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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}
Delphine K Farmer, Marina E Vance, Dustin Poppendieck, Jon Abbatt, Michael R Alves, Karen C Dannemiller, Cholaphan Deeleepojananan, Jenna Ditto, Brian Dougherty, Olivia R Farinas, Allen H Goldstein, Vicki H Grassian, Han Huynh, Deborah Kim, Jon C King, Jesse Kroll, Jienan Li, Michael F Link, Liora Mael, Kathryn Mayer, Andrew B Martin, Glenn Morrison, Rachel O'Brien, Shubhrangshu Pandit, Barbara J Turpin, Marc Webb, Jie Yu, Stephen M Zimmerman
{"title":"The chemical assessment of surfaces and air (CASA) study: using chemical and physical perturbations in a test house to investigate indoor processes.","authors":"Delphine K Farmer, Marina E Vance, Dustin Poppendieck, Jon Abbatt, Michael R Alves, Karen C Dannemiller, Cholaphan Deeleepojananan, Jenna Ditto, Brian Dougherty, Olivia R Farinas, Allen H Goldstein, Vicki H Grassian, Han Huynh, Deborah Kim, Jon C King, Jesse Kroll, Jienan Li, Michael F Link, Liora Mael, Kathryn Mayer, Andrew B Martin, Glenn Morrison, Rachel O'Brien, Shubhrangshu Pandit, Barbara J Turpin, Marc Webb, Jie Yu, Stephen M Zimmerman","doi":"10.1039/d4em00209a","DOIUrl":"10.1039/d4em00209a","url":null,"abstract":"<p><p>The Chemical Assessment of Surfaces and Air (CASA) study aimed to understand how chemicals transform in the indoor environment using perturbations (<i>e.g.</i>, cooking, cleaning) or additions of indoor and outdoor pollutants in a well-controlled test house. Chemical additions ranged from individual compounds (<i>e.g.</i>, gaseous ammonia or ozone) to more complex mixtures (<i>e.g.</i>, a wildfire smoke proxy and a commercial pesticide). Physical perturbations included varying temperature, ventilation rates, and relative humidity. The objectives for CASA included understanding (i) how outdoor air pollution impacts indoor air chemistry, (ii) how wildfire smoke transports and transforms indoors, (iii) how gases and particles interact with building surfaces, and (iv) how indoor environmental conditions impact indoor chemistry. Further, the combined measurements under unperturbed and experimental conditions enable investigation of mitigation strategies following outdoor and indoor air pollution events. A comprehensive suite of instruments measured different chemical components in the gas, particle, and surface phases throughout the study. We provide an overview of the test house, instrumentation, experimental design, and initial observations - including the role of humidity in controlling the air concentrations of many semi-volatile organic compounds, the potential for ozone to generate indoor nitrogen pentoxide (N<sub>2</sub>O<sub>5</sub>), the differences in microbial composition between the test house and other occupied buildings, and the complexity of deposited particles and gases on different indoor surfaces.</p>","PeriodicalId":74,"journal":{"name":"Environmental Science: Processes & Impacts","volume":" ","pages":""},"PeriodicalIF":4.3,"publicationDate":"2024-07-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141475474","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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}
Patrick M. Plehiers, Hans-Georg Pirkl, Lauren Ward and Christian Bögi
{"title":"Criteria for distinguishing heterogeneous from homogeneous conditions for aromatic diisocyanates in water†","authors":"Patrick M. Plehiers, Hans-Georg Pirkl, Lauren Ward and Christian Bögi","doi":"10.1039/D4EM00200H","DOIUrl":"10.1039/D4EM00200H","url":null,"abstract":"<p >Environmental fate and toxicity testing typically requires knowledge of the water solubility of the test substances. Determining the solubility of aromatic diisocyanates in water poses great challenges because of their hydrophobic nature and water-reactivity. The reactive dissolution process is dynamic and the establishment of a steady-state equilibrium cannot readily be observed. In preparation of experimental work, computer simulation was used to derive and evaluate criteria that enable distinguishing homogeneous (<em>i.e.</em>, substances would be fully dissolved in water) from heterogeneous (<em>i.e.</em>, a separate organic phase would be present) conditions. The simulation utilized available kinetic information and models representing the main physical and chemical processes taking place. It was found that the transition to heterogeneous conditions (<em>i.e.</em>, the exceedance of the solubility limit with increasing loading) can be identified by observing either a rapid decline in ultimate yield of the diamine hydrolysis product from near-stoichiometric to much lower values, or a decrease in rate of formation of the diamine hydrolysis product relative to its ultimate yield. The latter criterion is expected to be the more powerful indicator. These criteria can be used in future work to define and interpret an experimental program for determining solubility limits for aromatic diisocyanates or other poorly-soluble, water-reactive substances.</p>","PeriodicalId":74,"journal":{"name":"Environmental Science: Processes & Impacts","volume":" 8","pages":" 1373-1379"},"PeriodicalIF":4.3,"publicationDate":"2024-07-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141496394","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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}
{"title":"Critical review of fluorescence and absorbance measurements as surrogates for the molecular weight and aromaticity of dissolved organic matter†","authors":"Julie A. Korak and Garrett McKay","doi":"10.1039/D4EM00183D","DOIUrl":"10.1039/D4EM00183D","url":null,"abstract":"<p >Dissolved organic matter (DOM) is ubiquitous in aquatic environments and challenging to characterize due to its heterogeneity. Optical measurements (<em>i.e.</em>, absorbance and fluorescence spectroscopy) are popular characterization tools, because they are non-destructive, require small sample volumes, and are relatively inexpensive and more accessible compared to other techniques (<em>e.g.</em>, high resolution mass spectrometry). To make inferences about DOM chemistry, optical surrogates have been derived from absorbance and fluorescence spectra to describe differences in spectral shape (<em>e.g.</em>, E2:E3 ratio, spectral slope, fluorescence indices) or quantify carbon-normalized optical responses (<em>e.g.</em>, specific absorbance (SUVA) or specific fluorescence intensity (SFI)). The most common interpretations relate these optical surrogates to DOM molecular weight or aromaticity. This critical review traces the genesis of each of these interpretations and, to the extent possible, discusses additional lines of evidence that have been developed since their inception using datasets comparing diverse DOM sources or strategic endmembers. This review draws several conclusions. More caution is needed to avoid presenting surrogates as specific to either molecular weight or aromaticity, as these physicochemical characteristics are often correlated or interdependent. Many surrogates are proposed using narrow contexts, such as fractionation of a limited number of samples or dependence on isolates. Further study is needed to determine if interpretations are generalizable to whole-waters. Lastly, there is a broad opportunity to identify why endmembers with low abundance of aromatic carbon (<em>e.g.</em>, effluent organic matter, Antarctic lakes) often do not follow systematic trends with molecular weight or aromaticity as observed in endmembers from terrestrial environments with higher plant inputs.</p>","PeriodicalId":74,"journal":{"name":"Environmental Science: Processes & Impacts","volume":" 10","pages":" 1663-1702"},"PeriodicalIF":4.3,"publicationDate":"2024-06-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/em/d4em00183d?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141505200","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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}
Mohammad Qutob, Mohd Rafatullah, Syahidah Akmal Muhammad, Masoom Raza Siddiqui and Mahboob Alam
{"title":"A sustainable method for oxidizing phenanthrene in tropical soil using natural iron as a catalyst in a slurry phase reactor with persulfate assistance†","authors":"Mohammad Qutob, Mohd Rafatullah, Syahidah Akmal Muhammad, Masoom Raza Siddiqui and Mahboob Alam","doi":"10.1039/D4EM00328D","DOIUrl":"10.1039/D4EM00328D","url":null,"abstract":"<p >The presence of impurities is a significant restriction to the use of natural iron minerals as catalysts in the advanced oxidation process (AOP), especially if applied for soil remediation. This study evaluated the catalytic activity of tropical soil, which has relatively low impurities and naturally contains iron, for the remediation of phenanthrene (PHE) contamination. The system showed good performance, and the best result was 81% PHE removal after 24 h under experimental conditions of pH 7, [PHE]<small><sub>0</sub></small> = 300 mg/50 g soil, temperature 55 °C, air flow = 260 mL min<small><sup>−1</sup></small>, and [persulfate]<small><sub>0</sub></small> = 20 mg kg<small><sup>−1</sup></small>, while the mineralization was 61%. Nevertheless, certain limitations were noted in the soil matrix following the remediation procedure, including the appearance of cracks in the soil aggregate, reduction in the crystal size of the soil particles, and decline in the iron and aluminium contents. The results confirmed that the radicals play a major role in the remediation process. SO<small><sub>4</sub></small>˙<small><sup>−</sup></small> was more dominant than O<small><sub>2</sub></small>˙<small><sup>−</sup></small>, while HO˙ played a minor role. Additionally, the by-products were detected by gas chromatography-mass spectroscopy (GC-MS), and the degradation pathway of PHE is proposed. Toxicity assessment tests were performed by using a computational method. In spite of the challenges, this research achieved notable progress in soil remediation, taking a significant step forward in implementing the AOP without catalysts to activate oxidants and remove PHE within the soil. Also, this approach supports sustainability by reducing the need for extra materials and providing an environmentally friendly way of soil remediation.</p>","PeriodicalId":74,"journal":{"name":"Environmental Science: Processes & Impacts","volume":" 8","pages":" 1391-1404"},"PeriodicalIF":4.3,"publicationDate":"2024-06-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141505201","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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}
Giulia Kommana, Michael Hupfer, Jason Nicholas Woodhouse, Hans-Peter Grossart and Tobias Goldhammer
{"title":"Reduced greenhouse gas emissions from particulate organic matter degradation in iron-enriched sediments†","authors":"Giulia Kommana, Michael Hupfer, Jason Nicholas Woodhouse, Hans-Peter Grossart and Tobias Goldhammer","doi":"10.1039/D4EM00185K","DOIUrl":"10.1039/D4EM00185K","url":null,"abstract":"<p >Iron (Fe) plays an important role in the biogeochemical cycling of carbon and nutrients in aquatic systems. Reactive Fe phases can interact with organic carbon and facilitate the removal of carbon from the biogeochemical cycle; however, this important ecosystem function is often strongly controlled by Fe availability. Due to pollution from lignite mining in the Lusatian province in Northeast Germany, large amounts of iron and sulfate are released into the fluvial-lacustrine system of the Spree River. It was hypothesized that the input of freshly precipitated iron oxyhydroxides from mining areas (<em>e.g.</em>, ferrihydrite) alter the biodegradation of particulate organic matter (POM) in downstream lacustrine sediments. To investigate the Fe-dependent degradation of POM, slurries mimicking iron-polluted sediments (85 mg Fe per g, 116 mg Fe per g, and 149 mg Fe per g dry weight) were incubated with plankton or leaf POM under anoxic and oxic headspace conditions, and CO<small><sub>2</sub></small> and CH<small><sub>4</sub></small> emissions, water chemistry, and stable isotopes of dissolved inorganic carbon were measured. The experiments revealed that (i) with an increasing Fe content, the CO<small><sub>2</sub></small> and CH<small><sub>4</sub></small> emissions were gradually reduced, (ii) CO<small><sub>2</sub></small> and CH<small><sub>4</sub></small> production was higher during plankton degradation than during leaf decomposition, and (iii) under oxic conditions, CO<small><sub>2</sub></small> production was higher and CH<small><sub>4</sub></small> production was lower when compared to the treatments under anoxic conditions. These findings demonstrate that while benthic mineralization of fresh POM typically releases greenhouse gases into the water column, the availability of iron oxyhydroxides can contribute to reduced greenhouse gas emissions from sediments. This is of considerable relevance for future carbon budgets of similar mining-affected, iron-polluted fluvial-lacustrine river systems.</p>","PeriodicalId":74,"journal":{"name":"Environmental Science: Processes & Impacts","volume":" 7","pages":" 1227-1244"},"PeriodicalIF":4.3,"publicationDate":"2024-06-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141441818","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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}
Holly Barrett, Jianxian Sun, Yuhao Chen, Diwen Yang, Jonathan Verreault, Magali Houde, Frank Wania and Hui Peng
{"title":"Emerging investigator series: nontargeted screening of aryl hydrocarbon receptor agonists in endangered beluga whales from the St. Lawrence Estuary: beyond legacy contaminants†","authors":"Holly Barrett, Jianxian Sun, Yuhao Chen, Diwen Yang, Jonathan Verreault, Magali Houde, Frank Wania and Hui Peng","doi":"10.1039/D4EM00243A","DOIUrl":"10.1039/D4EM00243A","url":null,"abstract":"<p >The elevated concentrations of organohalogen contaminants in the endangered St. Lawrence Estuary (SLE) belugas have prompted the hypothesis that aryl hydrocarbon receptor (AhR) activity may be a contributor towards their potential adverse effects. While indirect associations between AhR and contaminant levels have been reported in SLE beluga tissues, AhR activity was never directly measured. Using bioassays and nontargeted analysis, this study contrasted AhR activity and agonist profiles between pooled tissue extracts of endangered SLE and non-threatened Arctic belugas. Tissue extracts of SLE belugas exhibited significantly higher overall AhR activity than that of Arctic belugas, with a 2000s SLE beluga liver extract exerting significantly higher activity than blubber extracts of SLE and Arctic belugas from the same time period. Contrary to our expectations, well-known AhR agonists detected by nontargeted analysis, including polychlorinated biphenyls (PCBs), were only minor contributors to the observed AhR activity. Instead, Tox21 suspect screening identified more polar chemicals, such as dyes and natural indoles, as potential contributors. Notably, the natural product bromoindole was selectively detected in SLE beluga liver at high abundance and was further confirmed as an AhR agonist. These findings highlighted the significance of the AhR-mediated toxicity pathway in belugas and underscored the importance of novel AhR agonists, particularly polar compounds, in its induction.</p>","PeriodicalId":74,"journal":{"name":"Environmental Science: Processes & Impacts","volume":" 9","pages":" 1451-1464"},"PeriodicalIF":4.3,"publicationDate":"2024-06-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141430961","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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}
Eva Rosendal Kjærgaard, Freja Hasager, Sarah Suda Petters, Marianne Glasius and Merete Bilde
{"title":"Bubble-mediated generation of airborne nanoplastic particles†","authors":"Eva Rosendal Kjærgaard, Freja Hasager, Sarah Suda Petters, Marianne Glasius and Merete Bilde","doi":"10.1039/D4EM00124A","DOIUrl":"10.1039/D4EM00124A","url":null,"abstract":"<p >Micro- and nanoplastic particles have been detected in most environmental compartments. The presence of microplastics in the remote marine atmosphere and close to large lakes suggests bubble mediated water–air transfer as a source of airborne microplastics, however, quantitative estimates of plastic emission from surface waters remain uncertain. In this work, we elucidate the emission of submicron polystyrene nanospheres by bubble bursting in a laboratory setting from low salinity waters (salinity 0–1.0 g kg<small><sup>−1</sup></small>), polystyrene particle diameter (103, 147 and 269 nm), aqueous particle number concentrations in the range 4 × 10<small><sup>7</sup></small>–2 × 10<small><sup>9</sup></small> cm<small><sup>−3</sup></small>, and bubble formation rate (0.88–3.35 L min<small><sup>−1</sup></small> of air). Production of polystyrene aerosols was demonstrated using a scanning mobility particle sizer and confirmed by analysis of filter samples using pyrolysis gas chromatography coupled to mass spectrometry. We show that production of polystyrene aerosol particles scales linearly with the number concentration of plastic particles in the water. Our results suggest that small amounts (0.01 g kg<small><sup>−1</sup></small>) of salt increase polystyrene particle production. To the best of our knowledge this is the first study of bubble mediated water–air transfer of plastic particles as small as 100 nm.</p>","PeriodicalId":74,"journal":{"name":"Environmental Science: Processes & Impacts","volume":" 7","pages":" 1216-1226"},"PeriodicalIF":4.3,"publicationDate":"2024-06-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141416643","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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}
{"title":"Kinetic study of isoprene hydroxy hydroperoxide radicals reacting with sulphur dioxide and their global-scale impact on sulphate formation†","authors":"Hiroo Hata and Kenichi Tonokura","doi":"10.1039/D4EM00232F","DOIUrl":"10.1039/D4EM00232F","url":null,"abstract":"<p >Isoprene is the most relevant volatile organic compound emitted during the biosynthesis of metabolism processes. The oxidation of isoprene by a hydroxy radical (OH) is one of the main consumption schemes that generate six isomers of isoprene hydroxy hydroperoxide radicals (ISOPOOs). In this study, the rate constants of ISOPOOs + sulphur dioxide (SO<small><sub>2</sub></small>) reactions that eventually generate sulphur trioxide (SO<small><sub>3</sub></small>), the precursor of sulphate aerosol (SO<small><sub>4</sub></small><small><sup>2−</sup></small>(p)), are determined using microcanonical kinetic theories coupled with molecular structures and energies estimated by quantum chemical calculations. The results show that the reaction rates range from 10<small><sup>−27</sup></small> to 10<small><sup>−20</sup></small> cm<small><sup>3</sup></small> molecule<small><sup>−1</sup></small> s<small><sup>−1</sup></small>, depending on the atmospheric temperature and structure of the six ISOPOO isomers. The effect of SO<small><sub>3</sub></small> formation from SO<small><sub>2</sub></small> oxidation by ISOPOOs on the atmosphere is evaluated by a global chemical transport model, along with the rate constants obtained from microcanonical kinetic theories. The results show that SO<small><sub>3</sub></small> formation is enhanced in regions with high SO<small><sub>2</sub></small> or low nitrogen oxide (NO), such as China, the Middle East, and Amazon rainforests. However, the production rates of SO<small><sub>3</sub></small> formation by ISOPOOs + SO<small><sub>2</sub></small> reactions are eight orders of magnitude lower than that from the OH + SO<small><sub>2</sub></small> reaction. This is indicative of SO<small><sub>4</sub></small><small><sup>2−</sup></small>(p) formation from the direct oxidation of SO<small><sub>2</sub></small> by ISOPOOs, which is almost negligible in the atmosphere. The results of this study entail a detailed analysis of SO<small><sub>3</sub></small> formation from gas-phase reactions of isoprene-derived products.</p>","PeriodicalId":74,"journal":{"name":"Environmental Science: Processes & Impacts","volume":" 7","pages":" 1147-1155"},"PeriodicalIF":4.3,"publicationDate":"2024-06-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/em/d4em00232f?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141295144","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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}