Mechanism of heterogeneous oxidation of carbonyl sulfide on AL2O3:: An in situ diffuse reflectance infrared Fourier transform spectroscopy investigation
Mechanism of heterogeneous oxidation of carbonyl sulfide on AL2O3:: An in situ diffuse reflectance infrared Fourier transform spectroscopy investigation
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DOI：
10.1021/jp055646y
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发表时间：
2006-02-23
影响因子：
3.3
通讯作者：
He, H
中科院分区：
文献类型：
--
作者：
Liu, JF;Yu, YB;He, H
利用原位漫反射红外傅立叶变换光谱（DRIFTS）研究了羰基硫化物（OCS）在不同类型氧化铝（Al2O3）表面298 K下的非均相反应。研究了氧化铝煅烧温度对其催化反应活性的影响。采用x射线衍射（XRD）和bruauer - emmet - teller （BET）方法对Al2O3的晶体结构和表面积进行了表征。结果表明，在298 K的温度下，吸附的OCS可在Al2O3表面催化氧化生成气相CO2和表面碳酸氢（HCO3-）和硫酸盐（SO42-）。Al2O3表面的羟基（OH）是OCS非均相氧化的关键反应物。此外，在热处理后的Al2O3表面可以观察到OCS与OH反应形成的中间产物硫代碳酸氢（HSCO2-）。在此基础上，探讨了OCS对Al2O3的非均相氧化反应机理。
Heterogeneous reaction of carbonyl sulfide (OCS) on the surface of different types of alumina (Al2O3) at 298 K was investigated in a closed system and a flowed system using in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS). The effects of calcination temperature of the Al2O3 on its catalyzed reactivity were studied. The crystal structure and surface area of the Al2O3 were characterized using X-ray diffraction (XRD) and the Brunauer-Emmett-Teller (BET) method. This paper revealed that adsorbed OCS could be catalytically oxidized on the surface of Al2O3 to form gas-phase CO2 and surface hydrogen carbonate (HCO3-) and sulfate (SO42-) species at 298 K. The surface hydroxyl (OH) species on the Al2O3 had been found to be the key reactant for the heterogeneous oxidation of OCS. Furthermore, the surface hydrogen thiocarbonate (HSCO2-) species, an intermediate formed in the reaction of OCS with OH, can be observed on the thermal-treated Al2O3. On the basis of these results, the reaction mechanism of heterogeneous oxidation of OCS on Al2O3 is discussed.