文献类型：期刊文献

英文题名：Phosphate-Functionalized CeO₂ Nanosheets for Efficient Catalytic Oxidation of Dichloromethane

作者：Dai, Qiguang[1];Zhang, Zhiyong[2];Yan, Jiaorong[1];Wu, Jinyan[1];Johnson, Grayson[2];Sun, Wei[1];Wang, Xingyi[1];Zhang, Sen[2];Zhan, Wangcheng[1]

机构：[1]East China Univ Sci & Technol, Key Lab Adv Mat, Res Inst Ind Catalysis, Sch Chem & Mol Engn, Shanghai 200237, Peoples R China;[2]Univ Virginia, Dept Chem, Charlottesville, VA 22904 USA

年份：2018

卷号：52

期号：22

起止页码：13430

外文期刊名：ENVIRONMENTAL SCIENCE & TECHNOLOGY

收录：;WOS:【SCI-EXPANDED(收录号:WOS:000451245700052)】；

基金：This work was supported by the National Key Research and Development Program of China (No. 2016YFC0204300), the National Natural Science Foundation of China (No. 21777043), and Jeffress Trust Awards Program in Interdisciplinary Research from Thomas F. and Kate Miller Jeffress Memorial Trust.

语种：英文

摘要：Tuning the nature and profile of acidic and basic sites on the surface of redox-active metal oxide nanostructures is a promising approach to constructing efficient catalysts for the oxidative removal of chlorinated volatile organic compounds (CVOCs). Herein, using dichloromethane (DCM) oxidation as a model reaction, we report that phosphate (POx) Bronsted acid sites can be incorporated onto a CeO2 nanosheet (NS) surface via an organophosphate-mediated route, which can effectively enhance the CeO2's catalytic performance by promoting the removal of chlorine poisoning species. From the systematic study of the correlation between POx composition, surface structure (acid and basic sites), and catalytic properties, we find that the incorporated Bronsted acid sites can also function to decrease the amount of medium-strong basic sites (O2-), reducing the formation of chlorinated organic byproduct monochloromethane (MCM) and leading to the desirable product, HCl. At the optimized P/Ce ratio (0.2), the POx-CeO2 NSs can perform a stable DCM conversion of 65-70% for over 10 h at 250 degrees C and over 95% conversion at 300 degrees C, superior to both pristine and other phosphate-modified CeO2 NSs. Our work clearly identifies the critical role of acid and basic sites over functionalized CeO2 for efficient catalytic CVOCs oxidation, guiding future advanced catalyst design for environmental remediation.