Heterogeneous reactions of sulfur dioxide on typical mineral particles

被引:133
作者
Zhang, Xingying
Zhuang, Guoshun [1 ]
Chen, Jianmin
Wang, Ying
Wang, Xiao
An, Zhisheng
Zhang, Peng
机构
[1] Fudan Univ, Dept Environm Sci & Engn, Ctr Atmospher Chem Study, Shanghai 200433, Peoples R China
[2] Beijing Normal Univ, Dept Chem, Ctr Atmospher Environm Study, Beijing 100875, Peoples R China
[3] Chinese Acad Sci, Inst Earth Environm, State Key Lab Loess & Quaternary Geol, Xian 710075, Peoples R China
[4] Chinese Acad Sci, Inst Atmospher Phys, NZC LAPC, Beijing 100029, Peoples R China
[5] China Meteorol Adm, Natl Satellite Meteorol Ctr, Key Lab Radiometr Calibrat & Validat Environm Sat, Beijing 100081, Peoples R China
关键词
D O I
10.1021/jp0617773
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
The heterogeneous reaction of SO2 on Al2O3, CaO, TiO2, MgO, FeOOH, Fe2O3, MnO2, and SiO2, as well as authentic aerosol sample, was investigated by using a White Cell coupled with in situ-FTIR and Diffuse Reflectance Infrared Fourier Transform Spectroscopy (DRIFTS). Simultaneous observations of reactants and products were performed to obtain full information on the mechanism and kinetics of the reactions. SO2 was irreversibly adsorbed to form surface sulfite (SO32-), bisulfite (HSO3-), and sulfate (SO42-). The reactivity order of these particles is the following: FeOOH > Al2O3 > mixture > MgO > Fe2O3 > SiO2. Field-collected aerosol showed significant activity for the oxidation of SO2. The uptake coefficient of SO2 on Al2O3 with different acidity varied in the order of basic Al2O3 > neutral Al2O3 > acidic Al2O3. The surface-active oxygen and hydroxyl might be the key factors for the conversion of SO2 to SO42-. The faster reaction rate could be achieved with greater surface area on particles with the same mass. On the basis of the same surface area Fe2O3 could be most reactive in the reaction with SO2 compared with all other particles. The apparent rate constants were determined to be 1.35 x 10(-2) and 9.4 x 10(-3) for uptake on Al2O3 and MgO, respectively, which are the same as the results of other scientists.
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页码:12588 / 12596
页数:9
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