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Effect of NOX, O3 and NH3 on sulfur isotope composition during heterogeneous oxidation of SO2: a laboratory investigation
Air Quality, Atmosphere & Health ( IF 5.1 ) Pub Date : 2024-03-09 , DOI: 10.1007/s11869-024-01543-0
Zhaobing Guo , Qingxiang Qian , Mingyi Xu , Bin Zhu , Qingjun Guo , Pengxiang Qiu

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.



中文翻译:

SO2 非均相氧化过程中 NOX、O3 和 NH3 对硫同位素组成的影响:实验室研究

硫酸盐气溶胶是雾霾的主要组成部分,在气溶胶形成和老化过程中发挥着重要作用。为了了解硫酸盐形成的机理,测定了二氧化硫在α-Fe 2 O 3表面的不同非均相氧化反应过程中硫同位素组成的特征。尽管NH 3更有利于硫酸盐的形成,但与NO X和O 3相比,34 S在NH 3存在下倾向于富集较轻的硫同位素。此外,考虑到NO X、O 3和NH 3在非均相氧化过程中潜在的竞争效应,通过瑞利蒸馏模型评估了每种气体的贡献。值得注意的是,NO X氧化占硫酸盐总产量的67.5±10%,从平均分馏因子来看,高于O 3 (13.3±10%)和NH 3 (19.2±10%)。由于硫酸盐形成过程中的硫同位素分馏,观察到的硫酸盐气溶胶的 δ 34 S 值与硫氧化率呈负相关。考虑到同位素质量平衡,随着SO 2氧化的进行,总体δ 34 S硫酸盐接近δ 34 S排放,这表明NO X在矿尘上SO 2的不同非均相氧化过程中发挥了主要作用,而不是唯一作用。表面。

更新日期:2024-03-11
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