文献类型：期刊文献

英文题名：Catalytic total oxidation of 1,2-dichloroethane over VOx/CeO2 catalysts: Further insights via isotopic tracer techniques

作者：Dai, Qiguang[1];Yin, Li-Li[2,3];Bai, Shuxing[1];Wang, Wei[1];Wang, Xingyi[1];Gong, Xue-Qing[2,3];Lu, Guanzhong[1]

机构：[1]E China Univ Sci & Technol, Res Inst Ind Catalysis, Key Lab Adv Mat, Shanghai 200237, Peoples R China;[2]E China Univ Sci & Technol, Ctr Computat Chem, Key Lab Adv Mat, Shanghai 200237, Peoples R China;[3]E China Univ Sci & Technol, Res Inst Ind Catalysis, Shanghai 200237, Peoples R China

年份：2016

卷号：182

起止页码：598

外文期刊名：APPLIED CATALYSIS B-ENVIRONMENTAL

收录：;EI(收录号：20154301449215);WOS:【SCI-EXPANDED(收录号:WOS:000365050700063)】；

基金：This work was supported by the National Natural Science Foundation of China (Nos. 21307033, 21277047, 21477036, 21322307, 21421004), Shanghai Natural Science Foundation (No. 13ZR1411000), Commission of Science and Technology of Shanghai Municipality (No. 11JC1402900), the National Basic Research Program of China (2011CB808505), the "Shu Guang" project of Shanghai Municipal Education Commission and Shanghai Education Development Foundation (13SG30) for financial support. The authors also thank the National Super Computing Center in Jinan for computing time.

语种：英文

外文关键词：CVOCs; Catalytic combustion; Surface hydroxyl group; Oxygen species; Isotopic tracer; Density Functional theory; Selective poisoning

摘要：Catalytic total oxidation of 1,2-dichloroethane (DCE) on CeO2 and VOx/CeO2 catalysts is investigated via various isotopic tracer techniques, including kinetic isotope effect (KIEs) measurements, in situ diffuse reflection infrared Fourier transform spectroscopy (DRIFT) of deuterated 1,2-dichloroethane oxidation, H/D exchange of surface hydroxyl groups, temperature-programmed isotopic exchange (TPIE) and O-18(2) isotope labeling experiments. The activation and dissociation of C-Cl bonds is determined to be the first step of DCE oxidation, and oxygen vacancies are identified as the main active sites by KIEs and density functional theory (DFT) calculations. For VOx/CeO2 catalysts, surface lattice oxygen is found to directly involve in oxidation of DCE via the formation of intermediate species of partial oxidation such as aldehyde species or CO, which are then totally oxidized into CO2 by the surface peroxide species. The occurrence of HCl is attributed to the reaction of surface hydroxyl groups with the dissociated Cl adsorbed on oxygen vacancies, whereas the rapid replenishment of the consumed OH is crucial for maintaining a better stability. (C) 2015 Elsevier B.V. All rights reserved.