{"title":"Effect of NOX, O3 and NH3 on sulfur isotope composition during heterogeneous oxidation of SO2: a laboratory investigation","authors":"Zhaobing Guo, Qingxiang Qian, Mingyi Xu, Bin Zhu, Qingjun Guo, Pengxiang Qiu","doi":"10.1007/s11869-024-01543-0","DOIUrl":null,"url":null,"abstract":"<div><p>Sulfate aerosol is a major fraction of haze, playing an important role in aerosol formation and aging processes. To understand the mechanism of sulfate formations, the characteristics of sulfur isotope composition were determined during different heterogeneous oxidation reactions of sulfur dioxide on the surface of α-Fe<sub>2</sub>O<sub>3</sub>. Although NH<sub>3</sub> was more beneficial to the formation of sulfate, compared with NO<sub>X</sub> and O<sub>3</sub>, <sup>34</sup>S tended to enrich the lighter sulfur isotopes in the presence of NH<sub>3</sub>. Furthermore, in consideration of the potential competitive effects of NO<sub>X</sub>, O<sub>3</sub>, and NH<sub>3</sub> in the heterogeneous oxidation processes, the contributions of each gas were evaluated via Rayleigh distillation model. Notably, the oxidation by NO<sub>X</sub> contributed 67.5±10 % of the whole sulfate production, which is higher than that of O<sub>3</sub> (13.3±10 %) and NH<sub>3</sub> (19.2±10 %) on the basic of the average fractionation factor. The observed δ<sup>34</sup>S values of sulfate aerosols were negatively correlated with sulfur oxidation ratios, owing to the sulfur isotopic fractionations during the sulfate formation processes. Given the isotope mass balance, the overall δ<sup>34</sup>S<sub>sulfate</sub> approached the δ<sup>34</sup>S<sub>emission</sub> as oxidation of SO<sub>2</sub> progressed, suggesting that NO<sub>X</sub> played a major rather than a sole role in the different heterogeneous oxidation processes of SO<sub>2</sub> on the mineral dust surface.</p></div>","PeriodicalId":49109,"journal":{"name":"Air Quality Atmosphere and Health","volume":null,"pages":null},"PeriodicalIF":2.9000,"publicationDate":"2024-03-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Air Quality Atmosphere and Health","FirstCategoryId":"93","ListUrlMain":"https://link.springer.com/article/10.1007/s11869-024-01543-0","RegionNum":4,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q3","JCRName":"ENVIRONMENTAL SCIENCES","Score":null,"Total":0}
引用次数: 0
Abstract
Sulfate aerosol is a major fraction of haze, playing an important role in aerosol formation and aging processes. To understand the mechanism of sulfate formations, the characteristics of sulfur isotope composition were determined during different heterogeneous oxidation reactions of sulfur dioxide on the surface of α-Fe2O3. Although NH3 was more beneficial to the formation of sulfate, compared with NOX and O3, 34S tended to enrich the lighter sulfur isotopes in the presence of NH3. Furthermore, in consideration of the potential competitive effects of NOX, O3, and NH3 in the heterogeneous oxidation processes, the contributions of each gas were evaluated via Rayleigh distillation model. Notably, the oxidation by NOX contributed 67.5±10 % of the whole sulfate production, which is higher than that of O3 (13.3±10 %) and NH3 (19.2±10 %) on the basic of the average fractionation factor. The observed δ34S values of sulfate aerosols were negatively correlated with sulfur oxidation ratios, owing to the sulfur isotopic fractionations during the sulfate formation processes. Given the isotope mass balance, the overall δ34Ssulfate approached the δ34Semission as oxidation of SO2 progressed, suggesting that NOX played a major rather than a sole role in the different heterogeneous oxidation processes of SO2 on the mineral dust surface.
期刊介绍：
Air Quality, Atmosphere, and Health is a multidisciplinary journal which, by its very name, illustrates the broad range of work it publishes and which focuses on atmospheric consequences of human activities and their implications for human and ecological health.
It offers research papers, critical literature reviews and commentaries, as well as special issues devoted to topical subjects or themes.
International in scope, the journal presents papers that inform and stimulate a global readership, as the topic addressed are global in their import. Consequently, we do not encourage submission of papers involving local data that relate to local problems. Unless they demonstrate wide applicability, these are better submitted to national or regional journals.
Air Quality, Atmosphere & Health addresses such topics as acid precipitation; airborne particulate matter; air quality monitoring and management; exposure assessment; risk assessment; indoor air quality; atmospheric chemistry; atmospheric modeling and prediction; air pollution climatology; climate change and air quality; air pollution measurement; atmospheric impact assessment; forest-fire emissions; atmospheric science; greenhouse gases; health and ecological effects; clean air technology; regional and global change and satellite measurements.
This journal benefits a diverse audience of researchers, public health officials and policy makers addressing problems that call for solutions based in evidence from atmospheric and exposure assessment scientists, epidemiologists, and risk assessors. Publication in the journal affords the opportunity to reach beyond defined disciplinary niches to this broader readership.
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