Unveiling Independent Catalytic Pathways of Dual-Active-Site Catalysts by Time-Resolved Spectroscopy of Reaction Intermediates

作者：Yuguang Jing, Xiaotian Zhou, Zhiyuan Wang, Zhongyi Liu, Chao Lu · 发表于：ACS Catalysis · 年份：2025 · DOI：10.1021/acscatal.5c05844 · 被引用次数：2 · 研究领域：Catalytic Processes in Materials Science、Catalysis and Oxidation Reactions、Electrocatalysts for Energy Conversion

Dual-active-site catalysts have been extensively applied in numerous fields. Currently, the widely accepted catalytic pathways of dual-active-site catalysts include synergistic catalysis, tandem catalysis, and single-site catalysis. However, these so-called catalytic pathways fail to dynamically decouple the competing reaction routes in multipathway systems with a single reactant, making it challenging to precisely regulate product selectivity. Therefore, it is of extreme significance to develop rapid and highly efficient strategies to deeply study the reaction pathways of dual-active-site catalysts for manipulating catalyst microstructure and distributing reaction products. In this contribution, we have leveraged time-resolved luminescence spectroscopy with subsecond temporal resolution to dynamically monitor the evolution of reactive intermediates to disclose the independent catalytic pathway for dual-active-site catalysts. It was revealed that the spatially isolated Ni 2+ -O v and O v -Ce 3+ dual sites in Ni/CeO 2 could drive acetone oxidation through two distinct parallel pathways: Ni 2+ -O v generated aldehyde intermediates (CH 3 CHO*) via weak oxygen activation, while the oxidation of O v -Ce 3 + enabled complete oxidation to CO 2 * through strong oxygen activation. The independent catalytic pathways of the dual-active site on Ni/CeO 2 were further demonstrated by regulating the propionaldehyde oxidation reaction. Our success would advance the rational design of dual-ac...