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Knudsen cell and smog chamber study of the heterogeneous uptake of sulfur dioxide on Chinese mineral dust

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Journal of Environmental Sciences 2014年第12期26卷 2423-2433页

作者： Li Zhou Weigang Wang Yanbo Gai Maofa Ge Beijing National Laboratory for Molecular Science (BNLMS) State Key Laboratory for Structural Chemistry of Unstable and Stable SpeciesInstitute of Chemistry Chinese Academy of Sciences Beijing National Laboratory for Molecular Science (BNLMS) State Key Laboratory for Structural Chemistry of Unstable and Stable SpeciesPeking University

The heterogeneous uptake processes of sulfur dioxide on two types of Chinese mineral dust（Inner Mongolia desert dust and Xinjiang sierozem） were investigated using both Knudsen cell and smog chamber system. The temperature dependence of the Uptake coefficients was studied over a range from 253 to 313 K using the Knudsen cell reactor, the initial Uptake coefficients decreased with the increasing of temperature for these two mineral dust samples, whereas the steady state Uptake coefficients of the Xinjiang sierozem increased with the temperature increasing, and these temperature dependence functions were obtained for the first time. In the smog chamber experiments at room temperature, the steady state Uptake coefficients of SO2 decreased evidently with the increasing of sulfur dioxide initial concentration from 1.72 × 1012 to 6.15 × 1012mol/cm3. Humid air had effect on the steady state Uptake coefficients of SO2 onto Inner Mongolia desert dust.Consequences about the understanding of the uptake processes onto mineral dust samples and the environmental implication were also discussed.

关键词： Mineral dust Sulfur dioxide Uptake coefficient Temperature dependence

Heterogeneous uptake of nitrogen dioxide on Chinese mineral dust

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Journal of Environmental Sciences 2015年第12期27卷 110-118页

作者： Li Zhou Weigang Wang Siqi Hou Shengrui Tong Maofa Ge Beijing National Laboratory for Molecular Science (BNLMS) State Key Laboratory for Structural Chemistry of Unstable and Stable SpeciesInstitute of ChemistryChinese Academy of Sciences Beijing National Laboratory for Molecular Science (BNLMS) State Key Laboratory for Structural Chemistry of Unstable and Stable SpeciesPeking University

Mineral dust is one of the major aerosols in the atmosphere.To assess its impact on trace atmospheric gases,in this work we present a laboratory study of the effect of temperature on the heterogeneous reaction of NO2 on the surface of ambient Chinese dust over the temperature range from 258 to 313 K.The results suggest that nitrogen dioxide could mainly be adsorbed on these types of Chinese mineral dust reversibly with little temperature dependence.Similar to a previous study on NO2 uptake on mineral aerosols,the Uptake coefficients are mainly on the order of 10^（-6） for the Chinese dust,when BET areas are taken into account.HONO was observed as a product,and its formation and decomposition on Chinese mineral dust during the uptake processes were also studied.The complete dataset from this study was compiled with previous literature determinations.Atmospheric implications of the heterogeneous reaction between NO2 and mineral dust are also discussed,in an effort to understand this important heterogeneous process.

关键词： Mineral dust Nitrogen dioxide Uptake coefficient Temperature dependence

Heterogeneous reaction of NO_2 on the surface of montmorillonite particles

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Journal of Environmental Sciences 2012年第10期24卷 1753-1758页

作者： Zefeng Zhang Jing Shang Tong Zhu Hongjun Li Defeng Zhao Yingju Liu Chunxiang Ye College of Environmental Sciences and Engineering Peking UniversityBeijing 100871China CMA Key Laboratory for Atmospheric Physics and Environment Nanjing University of Information Science and TechnologyNanjing 210044China

The studies on heterogeneous reactions over montmorillonite, which is a typical 2：1 layered aluminosilicate, will benefit to the Understanding of heterogeneous reactions on clay minerals. Montmorillonite can be classified as sodium montmorillonite or calcium montmorillonite depending on the cation presented between the different layers. Using diffuse reflectance infrared Fourier transform spectroscopy （DRIFTS）, the heterogeneous reaction mechanism of NO2 on the surface of montmorillonite was firstly investigated. Results showed that the reaction of NO2 on the surface of sodium and calcium montmorillonite fit a first-order kinetics, and the reaction duration of calcium montmorillonite was longer than that of sodium montmorillonite under the dry condition. For either sodium or calcium montmorillonite, the Uptake coefficient decreased as humidity increased.

关键词： heterogeneous reaction Uptake coefficient DRIFTS montmorillonite NO2