Preprints
https://doi.org/10.5194/acp-2020-506
https://doi.org/10.5194/acp-2020-506

  06 Jul 2020

06 Jul 2020

Review 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 Guo1, Mingyi Xu1, Yuxuan He1, Shuo Gao1, Chenmin Xu2, Bin Zhu3, Qingjun Guo4, Xiaoyu Shen1, Shuang Zhao1, and Pengxiang Qiu1 Zhaobing Guo et al.
  • 1Jiangsu Key Laboratory of Atmospheric Environment Monitoring and Pollution Control (AEMPC), Collaborative Innovation Center of Atmospheric Environment and Equipment Technology (CIC-AEET), School of Environmental Science and Engineering, Nanjing University of Information Science and Technology, Nanjing 210044, China
  • 2School of Environment, Nanjing Normal University, Nanjing 210023, China
  • 3School of Atmospheric Physics, Nanjing University of Information Science and Technology, Nanjing 210044, China
  • 4Insititude of Geographic Sciences and Natural Resources Research, Chinese Academy of Sciences, Beijing 100101, China

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.

Zhaobing Guo et al.

 
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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 et al.

Zhaobing Guo et al.

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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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