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

被引：105

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

来源：

APPLIED CATALYSIS B-ENVIRONMENTAL | 2016年 / 182卷

基金：

中国国家自然科学基金;

关键词：

CVOCs; Catalytic combustion; Surface hydroxyl group; Oxygen species; Isotopic tracer; Density Functional theory; Selective poisoning; MIXED-OXIDE CATALYSTS; VOLATILE ORGANIC-COMPOUNDS; INITIO MOLECULAR-DYNAMICS; DENSITY-FUNCTIONAL THEORY; AUGMENTED-WAVE METHOD; LOW-INDEX SURFACES; DEEP OXIDATION; CHLORINATED VOCS; CO OXIDATION; CEO2/H-ZSM5; CATALYSTS;

D O I：

10.1016/j.apcatb.2015.10.016

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：

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.

引用

页码：598 / 610

页数：13

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