Core–Shell Design of Metastable Phase Catalyst EnablesHighly-Performance Selective Hydrogenation
Jiaqi Su1, Yujin Ji2, Shize Geng1, Lamei Li1, Da Liu1, Hao Yu2, Beibei Song1, Youyong Li2,Chih-Wen Pao3, Zhiwei Hu4, Xiaoqing Huang5，* （黄小青）,Jianmei Lu1,*（路建美）, and Qi Shao1*（邵琪）
Adv. Mater. 2024, 36, 2308839
Abstract:Highly selective semihydrogenation of alkynes to alkenes is a highly important reaction for catalytic industry. Developing non-noble metal based catalysts with platinum group metal-like activity and selectivity is extremely crucial yet challenging. Metastable phase catalysts provide a potential candidate to realize high activity, yet the control of selectivity remains an open question. Here, this work first reports a metastable phase core-shell: face-centered cubic (fcc) phase Ag (10 at%) core-metastable hexagonal closest packed (hcp) phase Ni (90 at%) shell catalyst, which represents high conversion rate, high selectivity, and remarkable universality for the semihydrogenation of phenylacetylene and its derivatives. More impressively, a turnover frequency (TOF) value of 8241.8 h-1 is achieved, much higher than those of stable phase catalysts and reported platinum group metal based catalysts. Mechanistic investigation reveals that the surface of hcp Ni becomes more oxidized due to electron transfer from hcp Ni shell to fcc Ag core, which decreases the adsorption capacity of styrene on the metastable phase Ni surface, thus preventing full hydrogenation. This work has gained crucial research significance for the design of high performance metastable phase catalysts.
链接：//onlinelibrary.wiley.com/doi/10.1002/adma.202308839
