Atomic Three-Dimensional Investigations of Pd Nanocatalysts for Acetylene Semi-hydrogenation

• DOI: 10.1021/jacs.3c08619
• Publication Date: 2023-11-28T15:54:43Z
• Authors: Fan Xue; Qiang Li; Mingxin Lv; Yuanfei Song; Tianxing Yang; Xiaoge Wang; Tianyi Li; Yang Ren; Koji Ohara; Yufei He; Dianqing Li; Qiheng Li; Xin Chen; Kun Lin; Xianran Xing
• Keywords: Nanomaterial-based catalyst; Acetylene

Deciphering the three-dimensional (3D) insight into nanocatalyst surfaces at atomic level is crucial to understanding catalytic reaction mechanisms and developing high-performance catalysts. Nevertheless, better inherent insufficiency of a long-range ordered lattice in nanocatalysts big challenge. In this work, we report local structure Pd nanocatalysts, which beneficial for demonstrating shape-structure-adsorption relationship acetylene hydrogenation. The 5.27 nm spherical catalyst (Pdsph) shows an ethylene selectivity 88% complete conversion, much higher than those octahedron cube superior other reported monometallic so far. By virtue revelation combined with pair distribution function (PDF) reverse Monte Carlo (RMC) simulation, surface unique compressed strain Pd-Pd pairs Pdsph was revealed. Density functional theory calculations verified obvious weakening adsorption energy on account Pdsph. It main factor avoid over-hydrogenation acetylene. present entailing shape-induced manipulation 3D insight, opens new path understand optimize chemical activity heterogeneous catalysis process.