环境科学与技术最新文献

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Sediment Ballet: Unveiling the Dynamics of Metal Bioavailability in Sediments Following Resuspension and Reequilibration
IF 9.028 1区 环境科学与生态学
环境科学与技术 Pub Date : 2024-12-13 DOI: 10.1021/acs.est.4c08327
Dejin Xu, Haiyan Xiong, Qiuling Wu, Wenze Xiao, Stuart L. Simpson, Qiao-Guo Tan, Rong Chen, Minwei Xie
{"title":"Sediment Ballet: Unveiling the Dynamics of Metal Bioavailability in Sediments Following Resuspension and Reequilibration","authors":"Dejin Xu, Haiyan Xiong, Qiuling Wu, Wenze Xiao, Stuart L. Simpson, Qiao-Guo Tan, Rong Chen, Minwei Xie","doi":"10.1021/acs.est.4c08327","DOIUrl":"https://doi.org/10.1021/acs.est.4c08327","url":null,"abstract":"Assessing the risk of metal-contaminated sediments under disturbed conditions is challenging due to the lack of methods that capture instant changes in metal bioavailability. Existing approaches provide inadequate understandings of the processes regulating metal bioavailability under nonequilibrium conditions. Experiments were conducted to improve our understanding of the metal bioavailability dynamics induced by sediment resuspension and subsequent redeposition (reequilibration). An isotopically modified bioassay, a novel stable isotope tracing technique, was used to measure metal bioavailability (assimilation rates) to clams within short time windows. Changes in metal partitioning were characterized by porewater analysis using in situ extraction and the diffusive gradients in thin-films technique. Results showed that sediment resuspension released metals into porewater, while reequilibration scavenged metals from the porewater. The assimilation rates of Ni, Cu, and Pb increased with the resuspension time, aligning with increasing porewater concentrations. Unexpectedly, during reequilibration, the metal assimilation rates did not decrease. The discrepancies between bioavailability to the clam and porewater extrapolations may be due to differing sustained conditions of metals in sediments. Overall, this study unveils the metal bioavailability dynamics in nonequilibrium sediments, which could not be accurately predicted relying solely on porewater analysis. Incorporating rapid bioassays to determine bioavailability offers a valuable tool for robust ecological risk assessment.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"69 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2024-12-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142816172","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Insights into the Roles of Different Iron Species on Zeolites for N2O Selective Catalytic Reduction by CO
IF 9.028 1区 环境科学与生态学
环境科学与技术 Pub Date : 2024-12-13 DOI: 10.1021/acs.est.4c06924
Yunshuo Wu, Xuanhao Wu, Jie Fan, Haiqiang Wang, Zhongbiao Wu
{"title":"Insights into the Roles of Different Iron Species on Zeolites for N2O Selective Catalytic Reduction by CO","authors":"Yunshuo Wu, Xuanhao Wu, Jie Fan, Haiqiang Wang, Zhongbiao Wu","doi":"10.1021/acs.est.4c06924","DOIUrl":"https://doi.org/10.1021/acs.est.4c06924","url":null,"abstract":"Iron zeolites are promising candidates for mitigating nitrous oxide (N<sub>2</sub>O), a potent greenhouse gas and contributor to stratospheric ozone destruction. However, the atomic-level mechanisms by which different iron species, including isolated sites, clusters, and particles, participate in N<sub>2</sub>O decomposition in the presence of CO still remain poorly understood, which hinders the application of the reaction in practical technology. Herein, through experiments and density functional theory (DFT) calculations, we identified that isolated iron sites were active for N<sub>2</sub>O activation to generate adsorbed O* species, which readily reacted with CO following the Eley–Rideal (E-R) mechanism. In contrast, Fe<sub>2</sub>O<sub>3</sub> particles exhibited a different reaction pathway, directly reacting with CO to generate oxygen vacancies (O<sub>v</sub>), which could efficiently dissociate N<sub>2</sub>O following the Mars-van Krevelen (MvK) mechanism. Moreover, the transformation of iron oxide clusters into undercoordinated FeO<sub><i>x</i></sub> species by CO was also revealed through various techniques, such as CO-temperature-programmed reduction (TPR), and <i>ab initio</i> molecular dynamics (AIMD) simulations. Our study provides deeper insights into the roles of different iron species in N<sub>2</sub>O-SCR by CO, and is anticipated to facilitate the understanding of multicomponent catalysis and the design of efficient iron-containing catalysts for practical applications.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"7 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2024-12-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142816173","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Enhancing Ion Selectivity of Nanofiltration Membranes via Heterogeneous Charge Distribution
IF 9.028 1区 环境科学与生态学
环境科学与技术 Pub Date : 2024-12-13 DOI: 10.1021/acs.est.4c08841
Ruiqi Zheng, Shuyi Xu, Shifa Zhong, Xin Tong, Xin Yu, Yangying Zhao, Yongsheng Chen
{"title":"Enhancing Ion Selectivity of Nanofiltration Membranes via Heterogeneous Charge Distribution","authors":"Ruiqi Zheng, Shuyi Xu, Shifa Zhong, Xin Tong, Xin Yu, Yangying Zhao, Yongsheng Chen","doi":"10.1021/acs.est.4c08841","DOIUrl":"https://doi.org/10.1021/acs.est.4c08841","url":null,"abstract":"Nanofiltration technology holds significant potential for precisely separating monovalent and multivalent ions, such as lithium (Li) and magnesium (Mg) ions, during lithium extraction from salt lakes. This study bridges a crucial gap in understanding the impact of the membrane spatial charge distribution on ion-selective separation. We developed two types of mixed-charge membranes with similar pore sizes but distinct longitudinal and horizontal distributions of oppositely charged domains. The charge-mosaic membrane, synthesized and utilized for ion fractionation for the first time, achieved an exceptional water permeance of 15.4 LMH/bar and a Li/Mg selectivity of 108, outperforming the majority of published reports. Through comprehensive characterization, mathematical modeling, and machine learning methods, we provide evidence that the spatial charge distribution dominantly determines ion selectivity. The charge-mosaic structure excels by substantially promoting ion selectivity through locally enhanced Donnan effects while remaining unaffected by variations in feedwater concentration. Our findings not only demonstrate the applicability of charge-mosaic membranes to precise nanofiltration but also have profound implications for technologies demanding advanced ion selectivity, including those in the sustainable water treatment and energy storage industries.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"42 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2024-12-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142816174","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Challenges in Observation of Ultrafine Particles: Addressing Estimation Miscalculations and the Necessity of Temporal Trends
IF 9.028 1区 环境科学与生态学
环境科学与技术 Pub Date : 2024-12-13 DOI: 10.1021/acs.est.4c07460
Tzu-Chi Lin, Pei-Te Chiueh, Ta-Chih Hsiao
{"title":"Challenges in Observation of Ultrafine Particles: Addressing Estimation Miscalculations and the Necessity of Temporal Trends","authors":"Tzu-Chi Lin, Pei-Te Chiueh, Ta-Chih Hsiao","doi":"10.1021/acs.est.4c07460","DOIUrl":"https://doi.org/10.1021/acs.est.4c07460","url":null,"abstract":"Ultrafine particles (UFPs) pose a significant health risk, making comprehensive assessment essential. The influence of emission sources on particle concentrations is not only constrained by meteorological conditions but often intertwined with them, making it challenging to separate these effects. This study utilized valuable long-term particle number and size distribution (PNSD) data from 2018 to 2023 to develop a tree-based machine learning model enhanced with an interpretable component, incorporating temporal markers to characterize background or time series residuals. Our results demonstrated that, differing from PM<sub>2.5</sub>, which is significantly shaped by planetary boundary layer height, wind speed plays a crucial role in determining the particle number concentration (PNC), showing strong regional specificity. Furthermore, we systematically identified and analyzed anthropogenically influenced periodic trends. Notably, while Aitken mode observations are initially linked to traffic-related peaks, both Aitken and nucleation modes contribute to concentration peaks during rush hour periods on short-term impacts after deweather adjustment. Pollutant baseline concentrations are largely driven by human activities, with meteorological factors modulating their variability, and the secondary formation of UFPs is likely reflected in temporal residuals. This study provides a flexible framework for isolating meteorological effects, allowing more accurate assessment of anthropogenic impacts and targeted management strategies for UFP and PNC.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"10 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2024-12-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142816348","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Co-metabolic Biotransformation of Bisphenol AF by a Bisphenol A-Growing Bacterial Enrichment Culture
IF 9.028 1区 环境科学与生态学
环境科学与技术 Pub Date : 2024-12-12 DOI: 10.1021/acs.est.4c10861
Yiding Wu, Tianyue Yang, Yang Wu, Yi Liang, Xiangying Zeng, Zhiqiang Yu, Ping’an Peng
{"title":"Co-metabolic Biotransformation of Bisphenol AF by a Bisphenol A-Growing Bacterial Enrichment Culture","authors":"Yiding Wu, Tianyue Yang, Yang Wu, Yi Liang, Xiangying Zeng, Zhiqiang Yu, Ping’an Peng","doi":"10.1021/acs.est.4c10861","DOIUrl":"https://doi.org/10.1021/acs.est.4c10861","url":null,"abstract":"The fluorinated bisphenol A (2,2-bis[4-hydroxyphenyl]propane, BPA) substitute bisphenol AF (BPAF) could be more persistent and toxic than BPA, but little is known about its environmental fate. In this study, we established a co-metabolic BPAF-degrading bacterial enrichment culture with BPA as the growth substrate. BPAF degradation by the enrichment culture was dependent on BPA, and BPAF could be eliminated to below the detection limit with successive additions of BPA. BPAF was mainly degraded via phenolic ring hydroxylation and sequential ring cleavage, which are minor BPA transformation pathway. Conjugated BPAF products were also identified based on the characteristic CF<sub>3</sub><sup>–</sup> fragment and were found to accumulate during BPAF degradation. <i>Sphingopyxis</i> was the key BPA and BPAF degrader in the aerobic enrichment cultures, which was the most abundant genera in only BPA-added and BPA and BPAF-added cultures and was proven to be able to degrade BPA and BPAF by isolation. The aerobic co-metabolic BPAF degrading community also contain non-BPA and BPAF degraders, such as <i>Pandoraea</i>, which may play a supporting role in the community.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"28 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2024-12-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142809845","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
A Multidisciplinary Approach That Considers Occurrence, Geochemistry, Bioavailability, and Toxicity to Prioritize Critical Minerals for Environmental Research
IF 9.028 1区 环境科学与生态学
环境科学与技术 Pub Date : 2024-12-12 DOI: 10.1021/acs.est.4c11211
Sarah Jane O. White, Tyler J. Kane, Kate M. Campbell, Marie-Noële Croteau, Michael Iacchetta, Johanna M. Blake, Charles A. Cravotta, III, Bethany K. Kunz, Charles N. Alpers, Jill A. Jenkins, Katherine Walton-Day
{"title":"A Multidisciplinary Approach That Considers Occurrence, Geochemistry, Bioavailability, and Toxicity to Prioritize Critical Minerals for Environmental Research","authors":"Sarah Jane O. White, Tyler J. Kane, Kate M. Campbell, Marie-Noële Croteau, Michael Iacchetta, Johanna M. Blake, Charles A. Cravotta, III, Bethany K. Kunz, Charles N. Alpers, Jill A. Jenkins, Katherine Walton-Day","doi":"10.1021/acs.est.4c11211","DOIUrl":"https://doi.org/10.1021/acs.est.4c11211","url":null,"abstract":"Critical minerals (or critical elements) are minerals or elements that are essential to global security and development and have supply chains vulnerable to disruption. In general, knowledge of the environmental behavior and health effects of critical elements is needed to support the development of safe and environmentally responsible supplies. This knowledge includes identifying potential consequences of increased critical element production and use, alternative critical element sources such as mine wastes, and adverse effects of critical elements on ecosystem condition and organismal health. Here we identify significant data gaps in the understanding of critical elements in surficial and aquatic environments, and the need, given the large number of commodities (50) identified on the 2022 critical minerals list for the United States, for an approach to prioritize them for study of their environmental fate and effects. We propose a multidisciplinary approach for this prioritization, considering measures of occurrence, geochemistry, bioavailability, and toxicity. We describe relatively easy-to-obtain metrics for each of these topic areas and demonstrate the utility of this integrated prioritization approach using indium and zinc as examples. This approach facilitates prioritizing research with a focus on those critical elements that are most mobile in the environment, bioavailable, toxic, or simply lacking data in these categories.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"239 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2024-12-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142809846","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Correction to “Alternatives Exert Higher Health Risks Than Bisphenol A on Indo-Pacific Humpback Dolphins”
IF 9.028 1区 环境科学与生态学
环境科学与技术 Pub Date : 2024-12-12 DOI: 10.1021/acs.est.4c12912
Weifang Sun, Yongwei Guo, Xian Sun, Zhiwei Liu, Dingyu Luo, Nuoyan Huang, Zhuo Xu, Jiaxue Wu, Yuping Wu
{"title":"Correction to “Alternatives Exert Higher Health Risks Than Bisphenol A on Indo-Pacific Humpback Dolphins”","authors":"Weifang Sun, Yongwei Guo, Xian Sun, Zhiwei Liu, Dingyu Luo, Nuoyan Huang, Zhuo Xu, Jiaxue Wu, Yuping Wu","doi":"10.1021/acs.est.4c12912","DOIUrl":"https://doi.org/10.1021/acs.est.4c12912","url":null,"abstract":"Corrections to Figure 5C,E. Figure 5. Differentially expressed genes (DEGs) and KEGG pathway enrichment analysis of the transcriptome of ScSF exposed to BPA and its alternative. Volcano plots of DEGs (compared to the control group): (A) exposure to BPA; (C) exposure to BPP; (E) exposure to BPS; twenty most significantly enriched genes mapped by KEGG in (B) BPA, (D) BPP, and (F) BPS. This article has not yet been cited by other publications.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"29 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2024-12-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142809847","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Unravel the in-Source Fragmentation Patterns of Per- and Polyfluoroalkyl Substances during Analysis by LC-ESI-HRMS
IF 9.028 1区 环境科学与生态学
环境科学与技术 Pub Date : 2024-12-12 DOI: 10.1021/acs.est.4c08442
Ke Wang, Runyun Wang, Wenyu Shan, Zilin Yang, Yinjuan Chen, Lei Wang, Yanyan Zhang
{"title":"Unravel the in-Source Fragmentation Patterns of Per- and Polyfluoroalkyl Substances during Analysis by LC-ESI-HRMS","authors":"Ke Wang, Runyun Wang, Wenyu Shan, Zilin Yang, Yinjuan Chen, Lei Wang, Yanyan Zhang","doi":"10.1021/acs.est.4c08442","DOIUrl":"https://doi.org/10.1021/acs.est.4c08442","url":null,"abstract":"In-source fragmentation (ISF) was inevitable during electrospray ionization (ESI) of per- and polyfluoroalkyl substances (PFAS) when analyzed by liquid chromatography coupled with mass spectrometry (LC-MS), resulting in reduced response of molecular ions and misannotation of MS features. Herein, we analyzed 82 PFAS across 12 classes to systematically identify the structures with ISF potentials and reveal the fragmentation pathways. We found up to 100% ISF for 38 PFAS in six classes, which all contain the carboxylate (CO<sub>2</sub><sup>–</sup>) headgroup, including perfluoro(di)carboxylates (PF(di)CA), omega H/Cl substituted PFCA (ωH/Cl-PFCA), fluorotelomer carboxylates, and perfluoroalkyl ether carboxylates (PFECA). Seven ISF pathways were identified, including direct cleavage of C–CO<sub>2</sub><sup>–</sup>, C–O, and C–C bonds and eliminations of HF/CO<sub>2</sub>HF through cyclic transition states by the mechanisms of β-elimination, McLafferty rearrangement, or H···F bridging. We found that the loss of CO<sub>2</sub> is a prerequisite for most other pathways, explaining the absence of ISF for PFAS without a CO<sub>2</sub><sup>–</sup> headgroup. The elevated bond dissociation energy of C–CO<sub>2</sub><sup>–</sup> explained the reduced ISF for long-chain PFCA and ωH-PFCA. Raising the MS vaporizer and ion transfer tube temperatures significantly aggravated the ISF of most PFAS. These findings provide valuable references to inform the structural identification of PFAS and their degradation products.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"200 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2024-12-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142816178","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Engineering a Photoautotrophic Microbial Coculture toward Enhanced Biohydrogen Production
IF 9.028 1区 环境科学与生态学
环境科学与技术 Pub Date : 2024-12-12 DOI: 10.1021/acs.est.4c08629
Minmin Pan, Rodrigo Amarante Colpo, Stamatina Roussou, Chang Ding, Peter Lindblad, Jens O. Krömer
{"title":"Engineering a Photoautotrophic Microbial Coculture toward Enhanced Biohydrogen Production","authors":"Minmin Pan, Rodrigo Amarante Colpo, Stamatina Roussou, Chang Ding, Peter Lindblad, Jens O. Krömer","doi":"10.1021/acs.est.4c08629","DOIUrl":"https://doi.org/10.1021/acs.est.4c08629","url":null,"abstract":"The application of synthetic phototrophic microbial consortia holds promise for sustainable bioenergy production. Nevertheless, strategies for the efficient construction and regulation of such consortia remain challenging. Applying tools of genetic engineering, this study successfully constructed a synthetic community of phototrophs using <i>Rhodopseudomonas palustris</i> (<i>R. palustris</i>) and an engineered strain of <i>Synechocystis sp</i> PCC6803 for acetate production (<i>Synechocystis_acs</i>), enabling the production of biohydrogen and fatty acids during nitrogen and carbon dioxide fixation. Elemental balance confirmed carbon capture and nitrogen fixation into the consortium. The strategy of circadian illumination effectively limited oxygen levels in the system, ensuring the activity of the nitrogenase in <i>R. palustris</i>, despite oxygenic photosynthesis happening in <i>Synechocystis</i>. When infrared light was introduced into the circadian illumination, the production of H<sub>2</sub> (9.70 μmol mg<sup>–1</sup>) and fatty acids (especially C16 and C18) was significantly enhanced. Proteomic analysis indicated acetate exchange and light-dependent regulation of metabolic activities. Infrared illumination significantly stimulated the expression of proteins coding for nitrogen fixation, carbohydrate metabolism, and transporters in <i>R. palustris</i>, while constant white light led to the most upregulation of photosynthesis-related proteins in <i>Synechocystis_acs</i>. This study demonstrated the successful construction and light regulation of a phototrophic community, enabling H<sub>2</sub> and fatty acid production through carbon and nitrogen fixation.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"227 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2024-12-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142816227","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Chemical Composition of Secondary Organic Aerosol Formed from the Oxidation of Semivolatile Isoprene Epoxydiol Isomerization Products
IF 9.028 1区 环境科学与生态学
环境科学与技术 Pub Date : 2024-12-12 DOI: 10.1021/acs.est.4c06850
Molly Frauenheim, John Offenberg, Zhenfa Zhang, Jason D. Surratt, Avram Gold
{"title":"Chemical Composition of Secondary Organic Aerosol Formed from the Oxidation of Semivolatile Isoprene Epoxydiol Isomerization Products","authors":"Molly Frauenheim, John Offenberg, Zhenfa Zhang, Jason D. Surratt, Avram Gold","doi":"10.1021/acs.est.4c06850","DOIUrl":"https://doi.org/10.1021/acs.est.4c06850","url":null,"abstract":"3-Methylenebutane-1,2,4-triol and 3-methyltetrahydrofuran-2,4-diols, previously designated “C<sub>5</sub>-alkene triols”, were recently confirmed as in-particle isomerization products of isoprene-derived β-IEPOX isomers that are formed upon acid-driven uptake and partition back into the gas phase. In chamber experiments, we have systematically explored their gas phase oxidation by hydroxyl radical (<sup>•</sup>OH) as a potential source of secondary organic aerosol (SOA). <sup>•</sup>OH-initiated oxidation of both compounds in the presence of ammonium bisulfate aerosol resulted in substantial aerosol volume growth. Compositions of low-volatility products in both the gas and particulate phases were established by high-resolution mass spectrometry measurements. Under conditions mimicking the Southeast USA (50% relative humidity, bulk seed aerosol pH 1.4), we estimate the SOA yield from <sup>•</sup>OH-initiated oxidation of 3-methylenebutane-1,2,4-triol to be 93.1%, equating to 1.95 ± 0.81 Tg C Yr<sup>-1</sup>, and from 3-methyltetrahydrofuran-2,4-diol oxidation to be 26.7%, equating to 1.76 ± 1.26 Tg C Yr<sup>-1</sup>. Previously unreported isoprene-derived oxidation products, 2,3-dihydroxy-2-(hydroxymethyl)propanal, 1,3,4-trihydroxybutan-2-one, and four organosulfates have been confirmed in ambient SOA, and aid in understanding isoprene oxidation pathways in HO<sub>2</sub><sup>•</sup> dominated environments as NO<sub><i>x</i></sub> levels continue to decline in the US. This work underlines the need for inclusion of partitioning of in-particle formed semivolatile products and their atmospheric oxidation pathways in atmospheric models.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"5 1","pages":""},"PeriodicalIF":9.028,"publicationDate":"2024-12-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142816405","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
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