Preprints
https://doi.org/10.5194/acp-2020-506
https://doi.org/10.5194/acp-2020-506
06 Jul 2020
 | 06 Jul 2020
Status: this preprint was under review for the journal ACP but the revision was not accepted.

Effect of NOX, O3 and NH3 on sulfur isotope composition during heterogeneous oxidation of SO2: a laboratory investigation

Zhaobing Guo, Mingyi Xu, Yuxuan He, Shuo Gao, Chenmin Xu, Bin Zhu, Qingjun Guo, Xiaoyu Shen, Shuang Zhao, and Pengxiang Qiu

Abstract. Sulfate aerosol is a major fraction of haze, playing an important role in aerosol formation and aging processes. In order to understand the mechanism of sulfate formations, the characteristics of sulfur isotope composition were determined during different heterogeneous oxidation reactions of sulfur dioxide. 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, NOX oxidation contributed 67.5±10 % of the whole sulfate production, which is higher than O3 (13.3±10 %), and NH3 oxidation (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.

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Zhaobing Guo, Mingyi Xu, Yuxuan He, Shuo Gao, Chenmin Xu, Bin Zhu, Qingjun Guo, Xiaoyu Shen, Shuang Zhao, and Pengxiang Qiu
 
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Status: closed
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Status: closed
Status: closed
AC: Author comment | RC: Referee comment | SC: Short comment | EC: Editor comment
Printer-friendly Version - Printer-friendly version Supplement - Supplement
Zhaobing Guo, Mingyi Xu, Yuxuan He, Shuo Gao, Chenmin Xu, Bin Zhu, Qingjun Guo, Xiaoyu Shen, Shuang Zhao, and Pengxiang Qiu
Zhaobing Guo, Mingyi Xu, Yuxuan He, Shuo Gao, Chenmin Xu, Bin Zhu, Qingjun Guo, Xiaoyu Shen, Shuang Zhao, and Pengxiang Qiu

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Short summary
In order to gain insight into the formation mechanism of sulfate, stable sulfur isotope and Rayleigh distillation were applied to investigate the isotopic fractionations controlled by the oxidation pathways. The processes of SO2 oxidation on the surface of α-Fe2O3 with different chemical condition (NOX, O3 and NH3) were conducted in laboratory to study mechanism of SO2 oxidation. It was found that nitrogen oxides contributed primarily to the formation of sulfate among NOX, O3 and NH3 pathways.
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