Localized thermal levering events drive spontaneous kinetic oscillations during CO oxidation on Rh/Al2O3

作者：Donato Decarolis, Monik Panchal, Matthew G. Quesne, Khaled M. H. Mohammed, Shaojun Xu, Mark A. Isaacs, Adam H. Clark, Luke L. Keenan, Takuo Wakisaka, Kohei Kusada, Hiroshi Kitagawa, C. Richard A. Catlow, Emma K. Gibson, Alexandre Goguet, Peter P. Wells · 发表于：Nature Catalysis · 年份：2024 · DOI：10.1038/s41929-024-01181-w · 被引用次数：15 · 研究领域：Catalytic Processes in Materials Science、Catalysis and Oxidation Reactions、Advanced Chemical Physics Studies

Abstract Unravelling kinetic oscillations, which arise spontaneously during catalysis, has been a challenge for decades but is important not only to understand these complex phenomena but also to achieve increased activity. Here we show, through temporally and spatially resolved operando analysis, that CO oxidation over Rh/Al 2 O 3 involves a series of thermal levering events—CO oxidation, Boudouard reaction and carbon combustion—that drive oscillatory CO 2 formation. This catalytic sequence relies on harnessing localized temperature episodes at the nanoparticle level as an efficient means to drive reactions in situations in which the macroscopic conditions are unfavourable for catalysis. This insight provides a new basis for coupling thermal events at the nanoscale for efficient harvesting of energy and enhanced catalyst technologies.