Effect of O-Vacancy Concentration and Proximity on Electronic Metal-Support Interactions: Ru/ZrO2 Catalysts

被引：12
作者：
Li, Mengru [1 ]
Gross, Axel [1 ]
Behm, R. Juergen [1 ]
机构：
[1] Ulm Univ, Inst Theoret Chem, D-89081 Ulm, Germany
来源：
ACS CATALYSIS | 2022年 / 12卷 / 16期
关键词：
catalysis; adsorption; electronic metal-support interactions; DFT calculations; Ru; ZrO2; CO; TOTAL-ENERGY CALCULATIONS; CO OXIDATION; ACTIVE OXYGEN; ADSORPTION; METHANATION; TRANSITION; CLUSTERS; DENSITY; HYDROGENATION; STABILITY;
D O I：
10.1021/acscatal.2c03332
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：
Continuing our investigation of electronic metal-support interactions (EMSIs) in heterogeneous catalysis, we have investigated the effect of an increasing number of oxygen vacancies at the Ru-ZrO2 interface of supported Ru/ZrO2 catalysts on the CO adsorption properties. Employing density functional theory based calculations and using a model system consisting of a ZrO2(111) support and a Ru nanorod, we determined and discuss trends the O-vacancy formation energy in the interaction and charge transfer between support and Ru nanorod, in the local density of states on the Ru adsorption sites, and in the CO adsorption energy and in the C-O vibrational frequencies as a function of an increasing number of oxygen vacancies at the Ru-ZrO2 interface. Finally, we address consequences for our understanding of the role of EMSIs in heterogeneous catalysis and implications for the catalytic performance of realistic catalysts supported on reducible oxides.
引用
收藏
页码：10065 / 10079
页数：15
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