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Published on: July 28, 2020
Subsurface strain engineering in 3DOM-perovskites by noble metal single-atom substitution: Tuning oxygen vacancies
Xinrong Tian1, Yifan Li2, Ying Feng2
1Beijing Key Laboratory for Green Catalysis and Separation, State Key Laboratory of Materials Low-Carbon Recycling, Laboratory of Catalysis Chemistry and Nanoscience, Department of Chemical Engineering and Technology, College of Materials Science and Engineering, Beijing University of Technology, Beijing 100124, China; New Energy Engineering Department, Xingtai Polytechnic Institute of New Energy, Xingtai 055550, China.
Abstract:
Reducing methane emissions is the most direct and effective approach to mitigating rate of climate warming in the short term. This study enhances the catalytic activity of methane combustion by constructing lattice strain on the surface/subsurface of three-dimensionally ordered macroporous (3DOM) perovskites. The strain is primarily achieved through the solid-state reaction between multimetallic nanocrystals (PdMn or PdRhMn) and B-site deficient perovskites (LaCo0.95O3). The multimetallic nanocrystals are transformed into single noble metal atoms occupying the B-site, enabling controlled substitution on the surface or subsurface. This substitution induces lattice distortion and significant strain in the surface layer, profoundly affecting the oxygen vacancies and surface electronic structures of the perovskites, thereby improving its oxygen adsorption and activation capabilities. Consequently, the methane conversion efficiency is notably increased, with Pd1Mn/3DOM LaMnO3 and Pd1Rh1Mn/3DOM LaCoO3 showing the specific reaction rates at 300 °C of 9.1 and 125.5 µmol/(gPd·s), significantly higher than those (0.2 and 1.1 µmol/(gPd·s)) over Pd/3DOM LaMnO3 and Pd/3DOM LaCoO3, respectively.
