中国科学院化学所曹昌燕团队报道了加氢反应中由单原子密度诱导的Sabatier现象。相关研究成果发表在2023年5月26日出版的国际学术期刊《美国化学会杂志》。

Sabatier原理是多相催化中的一个基本概念，它为设计具有最高活性的最佳催化剂提供了指导。

该文首次报道了在原子尺度上由单原子密度引起的加氢反应中的一种新的Sabatier现象。研究人员通过P配位策略制备了一系列以Ir1-P4配位结构为主的Ir单原子催化剂（SACs），其密度范围为0.1-1.7原子/nm²。当用作氢化催化剂时，Ir单原子密度和氢化活性之间出现火山型关系，在0.7原子/nm²的中等密度处达到峰值。

机理研究表明，活化的H*在Ir单原子上的吸附和解吸强度之间的平衡是Sabatier现象的关键因素。这些Ir-SACs上转移的Bader电荷可作为解释结构-活性关系的描述符。此外，由于SACs中单个位点的几何和电子结构均匀，在使用优化的催化剂的化学选择性加氢反应中可以同时实现最大的活性和选择性。

该研究揭示了Sabatier原理，为合理设计更有效、更实用的氢化反应SACs提供了深刻的指导。

附：英文原文

Title: Sabatier Phenomenon in Hydrogenation Reactions Induced by Single-Atom Density

Author: Hongqiang Jin, Runqing Zhao, Peixin Cui, Xiaolong Liu, Jie Yan, Xiaohu Yu, Ding Ma, Weiguo Song, Changyan Cao

Issue&Volume: May 26, 2023

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

DOI: 10.1021/jacs.3c00786

Source: https://pubs.acs.org/doi/10.1021/jacs.3c00786