Size of cerium dioxide support nanocrystals dictates reactivity of highly dispersed palladium catalysts

• 成果类型: Article
• 署名作者: Muravev, Valery; Parastaev, Alexander; van den Bosch, Yannis; Ligt, Bianca; Claes, Nathalie; Bals, Sara; Kosinov, Nikolay; Hensen, Emiel J. M.
• 署名单位: Eindhoven University of Technology; University of Antwerp
• 刊物名称: SCIENCE
• ISSN/ISSBN: 0036-9681
• DOI: 10.1126/science.adf9082
• 发表日期: 2023-06-16
• 页码: 1174-1178
• 关键词: single-atom catalysts; co oxidation; active-sites; gold; ceo2; identification; clusters; nanoparticles; oxygen

摘要

The catalytic performance of heterogeneous catalysts can be tuned by modulation of the size and structure of supported transition metals, which are typically regarded as the active sites. In single-atom metal catalysts, the support itself can strongly affect the catalytic properties. Here, we demonstrate that the size of cerium dioxide (CeO2) support governs the reactivity of atomically dispersed palladium (Pd) in carbon monoxide (CO) oxidation. Catalysts with small CeO2 nanocrystals (similar to 4 nanometers) exhibit unusually high activity in a CO-rich reaction feed, whereas catalysts with medium-size CeO2 (similar to 8 nanometers) are preferred for lean conditions. Detailed spectroscopic investigations reveal support size-dependent redox properties of the Pd-CeO2 interface.