胺化
催化作用
化学
石墨烯
吸附
碳纤维
分子
介孔材料
功能群
基质(水族馆)
反应性(心理学)
无机化学
有机化学
组合化学
材料科学
纳米技术
复合数
医学
复合材料
病理
替代医学
聚合物
地质学
海洋学
作者
Xiangdong Long,Jia Wang,Guang Gao,Chao Nie,Peng Sun,Yongjie Xi,Fuwei Li
出处
期刊:ACS Catalysis
日期:2021-08-18
卷期号:11 (17): 10902-10912
被引量:10
标识
DOI:10.1021/acscatal.1c02264
摘要
Direct oxidative amination of the sp3 C–H bond is an attractive synthesis route to obtain amides. Conventional catalytic systems for this transformation are based on transition metals and complicated synthesis processes. Herein, direct and efficient oxidative amination of the methyl C–H bond in a wide range of N-heterocycles to access the corresponding amides over metal-free porous carbon is successfully developed. To understand the fundamental structure–activity relationships of carbon catalysts, the surface functional groups and the graphitization degree of porous carbon have been purposefully tailored through doping with nitrogen or phosphorus. The results of characterization, kinetic studies, liquid-phase adsorption experiments, and theoretical calculations indicate that the high activity of the carbon catalyst is attributed to the synergistic effect of surface acidic functional groups (hydroxyl/carboxylic acid/phosphate) and more graphene edge structures exposed on the surface of carbon materials with a high graphitization degree, in which the role of acidic functional groups is to adsorb the substrate molecule and the role of the graphene edge structure is to activate O2.
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