Direct Oxidative Amination of tlhe Methyl C–H Bond in N-Heterocycles over Meta-Free Mesoporous Carbon | |
Long Xiangdong1,2; Wang Jia1,2; Gao Guang2; Nie Chao2; Sun Peng2; Xi Yongjie2; Li Fuwei2 | |
刊名 | ACS Catalysis |
2021-08-17 | |
卷号 | 11期号:17页码:10902-10912 |
关键词 | heterogeneous catalysis oxidative amination amide porous carbon nitrogen-doped carbon phosphorus-doped carbon metal-free carbon catalyst |
DOI | 10.1021/acscatal.1c02264 |
英文摘要 | 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. |
语种 | 英语 |
内容类型 | 期刊论文 |
源URL | [http://ir.licp.cn/handle/362003/27684] |
专题 | 兰州化学物理研究所_OSSO国家重点实验室 |
通讯作者 | Li Fuwei |
作者单位 | 1.These authors contributed equally: Long Xiangdong, Wang Jia. 2.State Key Laboratory for Oxo Synthesis and Selective Oxidation, Lanzhou Institute of Chemical Physics, Chinese Academy of Sciences, Lanzhou 730000, China |
推荐引用方式 GB/T 7714 | Long Xiangdong,Wang Jia,Gao Guang,et al. Direct Oxidative Amination of tlhe Methyl C–H Bond in N-Heterocycles over Meta-Free Mesoporous Carbon[J]. ACS Catalysis,2021,11(17):10902-10912. |
APA | Long Xiangdong.,Wang Jia.,Gao Guang.,Nie Chao.,Sun Peng.,...&Li Fuwei.(2021).Direct Oxidative Amination of tlhe Methyl C–H Bond in N-Heterocycles over Meta-Free Mesoporous Carbon.ACS Catalysis,11(17),10902-10912. |
MLA | Long Xiangdong,et al."Direct Oxidative Amination of tlhe Methyl C–H Bond in N-Heterocycles over Meta-Free Mesoporous Carbon".ACS Catalysis 11.17(2021):10902-10912. |
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