Heterogeneous oxidation of carbonyl sulfide on mineral oxides  

作　　者：LIU YongChun LIU JunFeng HE Hong YU YunBo XUE Li 

机构地区：[1]Research Center for Eco-Environmental Science, Chinese Academy of Sciences, Beijing 100085, China

出　　处：《Chinese Science Bulletin》2007年第15期2063-2071,共9页

基　　金：the Ministry of Science and Technology of China (Grant No. 2007CB407301);the National Natural Science Foundation of China (Grant No. 20637001)

摘　　要：Heterogeneous oxidation of carbonyl sulfide (OCS) on mineral oxides including SiO2,Fe2O3,CaO,MgO,ZnO and TiO2,which are the main components of atmospheric particles,were investigated using in situ diffuse reflectance infrared Fourier transform spectroscopy (in situ DRIFTS),ion chromatography (IC),temperature-programmed desorption (TPD),X-ray diffraction (XRD) and Brunauer-Emmett-Teller (BET) methods. The main products and intermediates of the heterogeneous oxidation of OCS on these oxides were identified with in situ DRIFTS and IC. The reaction mechanism and kinetics were also discussed. It is found that the reaction mechanism on these mineral oxides is the same as that on Al2O3 for the same final products and the intermediates at room temperature. Namely,OCS can be catalytically oxidized to produce surface SO42- species and gaseous CO2 through the surface hydrogen thiocarbonate (HSCO2-) and HSO3- species. The activity series for heterogeneous oxidation of OCS follows: Al2O3 ≈ CaO > MgO > TiO2 ≈ ZnO > Fe2O3 > SiO2. The specific area,basic hydroxyl and surface basicity of these oxides have effect on the reactivity. This study suggests that heterogeneous reactions of OCS on mineral dust may be an unneglectable sink of OCS.Heterogeneous oxidation of carbonyl sulfide （OCS） on mineral oxides including SiO2, Fe2O3, CaO, MgO, ZnO and TiO2, which are the main components of atmospheric particles, were investigated using in situ diffuse reflectance infrared Fourier transform spectroscopy （in situ DRIFTS）, ion chromatography （IC）, temperature-programmed desorption （TPD）, X-ray diffraction （XRD） and Brunauer-Emmett-Teller （BET） methods. The main products and intermediates of the heterogeneous oxidation of OCS on these oxides were identified with in situ DRIFTS and IC. The reaction mechanism and kinetics were also discussed. It is found that the reaction mechanism on these mineral oxides is the same as that on Al2O3 for the same final products and the intermediates at room temperature. Namely, OCS can be catalytically oxidized to produce surface SO4^2- species and gaseous CO2 through the surface hydrogen thiocarbonate （HSCO2-） and HSO; species. The activity series for heterogeneous oxidation of OCS follows： Al2O3 ≈ CaO 〉 MgO 〉 TiO2 ≈ ZnO 〉 Fe2O3 〉 SiO2. The specific area, basic hydroxyl and surface basicity of these oxides have effect on the reactivity. This study suggests that heterogeneous reactions of OCS on mineral dust may be an unneglectable sink of OCS.

关 键 词：羰基硫化物 矿物氧化物 硫酸盐 反作用力 

分 类 号：O6[理学—化学]