巴豆醛
化学
位阻效应
选择性
催化作用
吸附
活动站点
Atom(片上系统)
光化学
分子
立体化学
结晶学
有机化学
计算机科学
嵌入式系统
作者
Yang Lou,Yongping Zheng,Xu Li,Na Ta,Jia Xu,Yifan Nie,Kyeongjae Cho,Jingyue Liu
摘要
Selective hydrogenation of unsaturated aldehydes to unsaturated alcohols is a valuable but challenging task for synthesizing fine chemicals. We report that single Rh atoms anchored to the edges of 2D MoS2 sheets can efficiently convert crotonaldehyde to crotyl alcohol with 100% selectivity via a steric confinement effect of pocketlike active sites. Characterization results suggest that the synthesized Rh1/MoS2 single-atom catalysts (SACs) possess a unique geometric and electronic configuration, which confines the adsorption mode of the reactant molecule by a steric effect. The DFT calculations suggest that the MoS2 sheets terminate with oxidized Mo edges and the Rh1 stably anchors at the Mo cation vacancy site, which can facilely dissociate H2 to H atoms. The dissociated H atoms spill over to react with the edge O atoms to form OH species and create an HO-Mo-Rh1-Mo-OH configuration, resembling a pocketlike active site, which confines the adsorption mode of the crotonaldehyde due to steric effects. Such specific adsorption configuration yields 100% selectivity. The strategy of constructing pocketlike active centers with single metal atoms and 2D nanosheets opens new approaches to designing highly selective SACs for specific classes of catalytic transformations.
科研通智能强力驱动
Strongly Powered by AbleSci AI