文献类型：期刊文献

英文题名：Impact of Aliovalent/Isovalent Ions (Gd, Zr, Pr, and Tb) on the Catalytic Stability of Mesoporous Ceria in the HCl Oxidation Reaction

作者：Cop, Pascal[1,2];Maile, Ruben[1,2];Sun, Yu[1,2,3];Khalid, Omeir[1,2];Djerdj, Igor[4];Esch, Patrick[5];Heiles, Sven[5];Over, Herbert[1,2];Smarsly, Bernd M.[1,2]

机构：[1]Justus Liebig Univ, Phys Chem Inst, D-35392 Giessen, Germany;[2]Justus Liebig Univ, Ctr Mat Res, D-35392 Giessen, Germany;[3]East China Univ Sci & Technol, Res Inst Ind Catalysis, Key Lab Adv Mat, Sch Chem & Mol Engn, Shanghai 200237, Peoples R China;[4]Josip Juraj Strossmayer Univ Osijek, Dept Chem, Osijek 31000, Croatia;[5]Justus Liebig Univ Giessen, Inst Inorgan & Analyt Chem, D-35392 Giessen, Germany

年份：2020

卷号：3

期号：8

起止页码：7406

外文期刊名：ACS APPLIED NANO MATERIALS

收录：;EI(收录号：20204109333793);WOS:【SCI-EXPANDED(收录号:WOS:000566778600011)】；

基金：The authors thank Tim Weber for the XPS measurements and Christian Sack for the help on the XPS analyses. The authors also thank Sebastian Werner, Kevin Turke, and Felix Badaczewski for the nitrogen physisorption measurements. The authors thank Bernhard Spengler for the ability to perform MP-AES measurements. I.Dj. acknowledges the support by the Croatian Science Foundation under project number PZS2019-02 2467.

语种：英文

外文关键词：mesoporous; ceria; doped; praseodymium; stability; OSC; HCl oxidation

摘要：CeO2 is a promising material in the catalytic recovery of Cl-2 from HCl by oxidation with O-2 due to its beneficial redox properties (Ce3+/Ce4+) and accompanied oxygen storage capacity (OSC). Two options to tailor the OSC are the usage of dopants and nanostructuring. In this work, we report the synthesis of mesoporous doped Ce0.9M0.1O2 (M = Zr, Gd, Pr, and Tb) powders with identical mesopore size, shape, and specific surface area (approximate to 90 m(2) g(-1)) to investigate the impact of aliovalent (Gd), isovalent (Zr), and aliovalent/isovalent (Pr and Tb) dopants on the OSC as well as on the catalytic activity/stability. The cubic arrangement of spherical 12 nm mesopores surrounded by a crystalline framework is obtained by using a diblock copolymer as structure directing agent in the sol-gel-based preparation approach, indicated by small angle X-ray scattering (SAXS) and scanning electron microscopy (SEM). Pr-doped CeO2 revealed the highest oxygen storage capacity but the lowest catalytic activity/stability in the HCl oxidation together with the Tb- and Gd-doped samples. By contrast, the Zr-doped mesoporous CeO2 powders showed the highest catalytic performance and stability in the CO and HCl oxidation of all samples but a lower OSC. These findings suggest that the OSC should therefore be treated with caution when relating to the catalytic performance in oxidation reactions. The differences in the stability are in agreement with recent studies of the HCl oxidation on model cerium oxide films with defined stoichiometry: the low stability of the aliovalent doped CeO2 materials in the HCl oxidation reaction can be attributed to a large number of oxygen vacancies.