文献类型：期刊文献

英文题名：sReactivation of CeO2-based Catalysts in the HCl Oxidation Reaction:In situQuantification of the Degree of Chlorination and Kinetic Modeling

作者：Sun, Yu[1,2];Hess, Franziska[3,4];Djerdj, Igor[5];Wang, Zheng[1,2];Weber, Tim[2,6];Guo, Yanglong[1];Smarsly, Bernd M.[2,6];Over, Herbert[2,6]

机构：[1]East China Univ Sci & Technol, Key Lab Adv Mat, Res Inst Ind Catalysis, Shanghai 200237, Peoples R China;[2]Justus Liebig Univ, Phys Chem Inst, Heinrich Buff Ring 17, D-35392 Giessen, Germany;[3]Rhein Westfal TH Aachen, Inst Phys Chem, Landoltweg 2, D-52074 Aachen, Germany;[4]Tech Univ Berlin, Inst Chem, Str 17 Juni 124, D-10623 Berlin, Germany;[5]JJ Strossmayer Univ Osijek, Dept Chem, Ul Cara Hadrijana 8-a, HR-31000 Osijek, Croatia;[6]Justus Liebig Univ, Zentrum Materialforsch, Heinrich Buff Ring 16, D-35392 Giessen, Germany

年份：2020

卷号：12

期号：21

起止页码：5511

外文期刊名：CHEMCATCHEM

收录：;EI(收录号：20203709165212);WOS:【SCI-EXPANDED(收录号:WOS:000567495600001)】；

基金：This work was supported by the National Key Research and Development Program of China (2016YFC0204300), National Natural Science Foundation of China (21577035), Commission of Science and Technology of Shanghai Municipality (13521103402, 15DZ1205305) and 111 Project (B08021). Yu Sun gratefully acknowledge the China Scholarship Council for the Joint-Ph.D program between the Research Institute of Industrial Catalysis of East China University of Science and Technology and the Physical Chemistry Institute of Justus-Liebig-University Giessen. We acknowledge support from the Laboratory of Materials Research at the JLU. Franziska Hess acknowledges funding by Fond der Chemischen Industrie in the form of a Liebig fellowship (Li 204/02). Open access funding enabled and organized by Projekt DEAL.

语种：英文

外文关键词：Deacon reaction; stability; reactivation; in situexperiment; Avrami modelling

摘要：Deactivation of CeO2-based catalysts in the HCl oxidation reaction proceeds via selective bulk chlorination of the active CeO(2)component to form CeCl(3)xnH(2)O. We study the reactivation of two bulk-chlorinated CeO2-based Deacon catalysts by oxygen treatment at 430 degrees C, namely pure CeO(2)and 20 mol % of CeO(2)supported on preformed ZrO(2)particles (20CeO(2)@ZrO2), with a dedicated experiment. In the flow reactor setup we determinein-situthe degree of chlorination of the catalyst by quantifying down-stream with in-situ UV-Vis spectroscopy the total amount of chlorine in the catalyst that is exchanged by reoxidation at 430 degrees C. The activity of deactivated 20CeO(2)@ZrO(2)can be fully restored by oxygen exposure at 430 degrees C, while that of pure CeO(2)declines steadily. Since the UV-Vis analytics is fast and sensitive, we can follow the kinetics of reoxidation. To rationalize the observed kinetics, we develop a modified Johnson-Mehl-Avrami-Kolmogorov (JMAK) model based on a nucleation-and-growth approach for the reoxidation of the catalyst starting from the chlorinated phase. The fast reoxidation kinetics of chlorinated 20CeO(2)@ZrO(2)is traced to a fast nucleation rate.