Heterogeneous Reaction of SO2 on Manganese Oxides: the Effect of Crystal Structure and Relative Humidity

Abstract Manganese oxides from anthropogenic sources can promote the formation of sulfate through catalytic oxidation of SO2. In this study, the kinetics of SO2 reactions on MnO2 with different morphologies (α, β, γ and δ) was investigated using flow tube reactor and in situ Diffuse Reflectance Infr...

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Autores principales:	Weiwei Yang, Jianghao Zhang, Qingxin Ma, Yan Zhao, Yongchun Liu, Hong He
Formato:	article
Lenguaje:	EN
Publicado:	Nature Portfolio 2017
Materias:	Medicine R Science Q
Acceso en línea:	https://doaj.org/article/55a2cd0b4ef04beb9456d136d732cd05
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spelling	oai:doaj.org-article:55a2cd0b4ef04beb9456d136d732cd052021-12-02T16:06:59ZHeterogeneous Reaction of SO2 on Manganese Oxides: the Effect of Crystal Structure and Relative Humidity10.1038/s41598-017-04551-62045-2322https://doaj.org/article/55a2cd0b4ef04beb9456d136d732cd052017-07-01T00:00:00Zhttps://doi.org/10.1038/s41598-017-04551-6https://doaj.org/toc/2045-2322Abstract Manganese oxides from anthropogenic sources can promote the formation of sulfate through catalytic oxidation of SO2. In this study, the kinetics of SO2 reactions on MnO2 with different morphologies (α, β, γ and δ) was investigated using flow tube reactor and in situ Diffuse Reflectance Infrared Fourier Transform Spectroscopy (DRIFTS). Under dry conditions, the reactivity towards SO2 uptake was highest on δ-MnO2 but lowest on β-MnO2, with a geometric uptake coefficient (γobs) of (2.42 ± 0.13) ×10–2 and a corrected uptake coefficient (γc) of (1.48 ± 0.21) ×10−6 for the former while γobs of (3.35 ± 0.43) ×10−3 and γc of (7.46 ± 2.97) ×10−7 for the latter. Under wet conditions, the presence of water altered the chemical form of sulfate and was in favor for the heterogeneous oxidation of SO2. The maximum sulfate formation rate was reached at 25% RH and 45% for δ-MnO2 and γ-MnO2, respectively, possibly due to their different crystal structures. The results suggest that morphologies and RH are important factors influencing the heterogeneous reaction of SO2 on mineral aerosols, and that aqueous oxidation process involving transition metals of Mn might be a potential important pathway for SO2 oxidation in the atmosphere.Weiwei YangJianghao ZhangQingxin MaYan ZhaoYongchun LiuHong HeNature PortfolioarticleMedicineRScienceQENScientific Reports, Vol 7, Iss 1, Pp 1-14 (2017)
institution	DOAJ
collection	DOAJ
language	EN
topic	Medicine R Science Q
spellingShingle	Medicine R Science Q Weiwei Yang Jianghao Zhang Qingxin Ma Yan Zhao Yongchun Liu Hong He Heterogeneous Reaction of SO2 on Manganese Oxides: the Effect of Crystal Structure and Relative Humidity
description	Abstract Manganese oxides from anthropogenic sources can promote the formation of sulfate through catalytic oxidation of SO2. In this study, the kinetics of SO2 reactions on MnO2 with different morphologies (α, β, γ and δ) was investigated using flow tube reactor and in situ Diffuse Reflectance Infrared Fourier Transform Spectroscopy (DRIFTS). Under dry conditions, the reactivity towards SO2 uptake was highest on δ-MnO2 but lowest on β-MnO2, with a geometric uptake coefficient (γobs) of (2.42 ± 0.13) ×10–2 and a corrected uptake coefficient (γc) of (1.48 ± 0.21) ×10−6 for the former while γobs of (3.35 ± 0.43) ×10−3 and γc of (7.46 ± 2.97) ×10−7 for the latter. Under wet conditions, the presence of water altered the chemical form of sulfate and was in favor for the heterogeneous oxidation of SO2. The maximum sulfate formation rate was reached at 25% RH and 45% for δ-MnO2 and γ-MnO2, respectively, possibly due to their different crystal structures. The results suggest that morphologies and RH are important factors influencing the heterogeneous reaction of SO2 on mineral aerosols, and that aqueous oxidation process involving transition metals of Mn might be a potential important pathway for SO2 oxidation in the atmosphere.
format	article
author	Weiwei Yang Jianghao Zhang Qingxin Ma Yan Zhao Yongchun Liu Hong He
author_facet	Weiwei Yang Jianghao Zhang Qingxin Ma Yan Zhao Yongchun Liu Hong He
author_sort	Weiwei Yang
title	Heterogeneous Reaction of SO2 on Manganese Oxides: the Effect of Crystal Structure and Relative Humidity
title_short	Heterogeneous Reaction of SO2 on Manganese Oxides: the Effect of Crystal Structure and Relative Humidity
title_full	Heterogeneous Reaction of SO2 on Manganese Oxides: the Effect of Crystal Structure and Relative Humidity
title_fullStr	Heterogeneous Reaction of SO2 on Manganese Oxides: the Effect of Crystal Structure and Relative Humidity
title_full_unstemmed	Heterogeneous Reaction of SO2 on Manganese Oxides: the Effect of Crystal Structure and Relative Humidity
title_sort	heterogeneous reaction of so2 on manganese oxides: the effect of crystal structure and relative humidity
publisher	Nature Portfolio
publishDate	2017
url	https://doaj.org/article/55a2cd0b4ef04beb9456d136d732cd05
work_keys_str_mv	AT weiweiyang heterogeneousreactionofso2onmanganeseoxidestheeffectofcrystalstructureandrelativehumidity AT jianghaozhang heterogeneousreactionofso2onmanganeseoxidestheeffectofcrystalstructureandrelativehumidity AT qingxinma heterogeneousreactionofso2onmanganeseoxidestheeffectofcrystalstructureandrelativehumidity AT yanzhao heterogeneousreactionofso2onmanganeseoxidestheeffectofcrystalstructureandrelativehumidity AT yongchunliu heterogeneousreactionofso2onmanganeseoxidestheeffectofcrystalstructureandrelativehumidity AT honghe heterogeneousreactionofso2onmanganeseoxidestheeffectofcrystalstructureandrelativehumidity
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Heterogeneous Reaction of SO2 on Manganese Oxides: the Effect of Crystal Structure and Relative Humidity

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