文献类型：期刊文献

英文题名：Shape-Controlled CeO2 Nanoparticles: Stability and Activity in the Catalyzed HCl Oxidation Reaction

作者：Li, Chenwei[1,2];Sun, Yu[1];Djerdj, Igor[3];Voepel, Pascal[2];Sack, Carl-Christian[2];Weller, Tobias[2];Ellinghaus, Ruediger[2];Sann, Joachim[2];Guo, Yanglong[1];Smarsly, Bernd M.[2];Over, Herbert[2]

机构：[1]East China Univ Sci & Technol, Sch Chem & Mol Engn, Res Inst Ind Catalysis, Key Lab Adv Mat, Shanghai 200237, Peoples R China;[2]Justus Liebig Univ, Phys Chem Inst, Heinrich Buff Ring 17, D-35392 Giessen, Germany;[3]JJ Strossmayer Univ Osijek, Dept Chem, Ulica Cara Hadrijana 8-A, HR-31000 Osijek, Croatia

年份：2017

卷号：7

期号：10

起止页码：6453

外文期刊名：ACS CATALYSIS

收录：;EI(收录号：20174504369535);WOS:【SCI-EXPANDED(收录号:WOS:000412795700009)】；

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). C.L. gratefully acknowledges the China Scholarship Council for the Joint-Ph.D program between the China Scholarship Council and the Physikalisch-Chemisches Institut of Justus-Liebig-University Giessen. We acknowledge financial support by the LOEWE program STORE-E within the Center for Materials Research at the JLU.

语种：英文

外文关键词：Deacon process; CeO2; shape controlled particles; structure sensitivity; stability; activity

摘要：CeO2 is a promising catalyst for the HCl oxidation (Deacon process) in order to recover Cl-2. Employing shape-controlled CeO2 nanoparticles (cubes, octahedrons, rods) with facets of preferential orientations ((100), (111), (110)), we studied the activity and stability under two reaction conditions (harsh: Ar:HCl:O-2 = 6:2:2 and mild: Ar:HCl:O-2 = 7:1:2). It turns out that both activity and stability are structure-sensitive. In terms of space time yield (STY), the rods are the most active particles, followed by the cubes and finally the octahedrons. This very same trend is reconciled with the complete oxygen storage capacity (OSCc), indicating a correlation between the observed activity STY and the OSCc. The apparent activation energies are about 50 kJ/mol for cubes and rods, while the octahedrons reveal an apparent activation energy of 65 kJ/mol. The reaction order in O-2 is positive (0.260.32). Under mild reaction conditions, all three morphologies are stable, consistent with corresponding studies of CeO2 powders and CeO2 nanofibers. Under harsh reaction conditions, however, cubes and octahedrons are both instable, forming hydrated CeCl3, while rods are still stable. The present stability and activity experiments in the catalytic HCl oxidation reaction over shape-controlled CeO2 nanoparticles may serve as benchmarks for future ab initio studies of the catalyzed HCl oxidation reaction over well-defined CeO2 surfaces.