Sabatier Phenomenon in Hydrogenation Reactions Induced by Single-Atom Density

• DOI: 10.1021/jacs.3c00786
• Publication Date: 2023-05-26T12:37:56Z
• Authors: Hongqiang Jin; Runqing Zhao; Peixin Cui; Xiaolong Liu; Jie Yan; Xiaohu Yu; Ding Ma; Weiguo Song; Changyan Cao

The Sabatier principle is a fundamental concept in heterogeneous catalysis that provides guidance for designing optimal catalysts with the highest activities. For first time, we here report new phenomenon hydrogenation reactions induced by single-atom density at atomic scale. We produce series of Ir (SACs) predominantly Ir1-P4 coordination structure densities ranging from 0.1 to 1.7 atoms/nm2 through P-coordination strategy. When used as hydrogenation, volcano-type relationship between and activity emerges, summit moderate 0.7 atoms/nm2. Mechanistic studies show balance adsorption desorption strength activated H* on single atoms found be key factor phenomenon. transferred Bader charge these SACs proposed descriptor interpret structure-activity relationship. In addition, maximum selectivity can simultaneously achieved chemoselective optimized catalyst due uniform geometric electronic structures sites SACs. present study reveals an insightful rational design more efficient practicable reactions.