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Heterogeneous oxidation of carbonyl sulfide on mineral oxides

机译：矿物氧化物上羰基硫的非均相氧化

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摘要

Heterogeneous oxidation of carbonyl sulfide (OCS) on mineral oxides including SiO_2, Fe_2O_3, CaO, MgO, ZnO and TiO_2, 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 Al_2O_3 for the same final products and the intermediates at room temperature. Namely, OCS can be catalytically oxidized to produce surface SO_4~(2-) species and gaseous CO_2 through the surface hydrogen thiocarbonate (HSCO_2~-) and HSO_3~- species. The activity series for heterogeneous oxidation of OCS follows: Al_2O_3 ≈ CaO> MgO > TiO_2 ≈ ZnO > Fe_2O_3 > SiO_2. 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.
机译：使用原位漫反射红外傅里叶变换光谱法（原位DRIFTS）研究了大气颗粒物的主要成分SiO_2，Fe_2O_3，CaO，MgO，ZnO和TiO_2等矿物氧化物上羰基硫化物（OCS）的非均相氧化，离子色谱（IC），程序升温脱附（TPD），X射线衍射（XRD）和Brunauer-Emmett-Teller（BET）方法。用原位DRIFTS和IC鉴定了OCS在这些氧化物上进行多相氧化的主要产物和中间体。还讨论了反应机理和动力学。发现在室温下，相同的最终产物和中间体在这些矿物氧化物上的反应机理与在Al_2O_3上的反应机理相同。即，OCS可以通过表面硫代碳酸氢盐（HSCO_2〜-）和HSO_3〜-种类被催化氧化以产生表面SO_4〜（2-）种类和气态CO_2。 OCS异质氧化的活性序列为：Al_2O_3≈CaO> MgO> TiO_2≈ZnO> Fe_2O_3> SiO_2。这些氧化物的比表面积，碱性羟基和表面碱性对反应性有影响。这项研究表明，OCS对矿物粉尘的异质反应可能是OCS不可忽视的汇。

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