Direct Oxidative Amination of tlhe Methyl C–H Bond in N-Heterocycles over Meta-Free Mesoporous Carbon | |
Department | 羰基合成与选择氧化国家重点实验室(OSSO) |
Long Xiangdong1,2; Wang Jia1,2; Gao Guang1; Nie Chao1; Sun Peng1; Xi Yongjie1; Li Fuwei1 | |
The second department | 清洁催化与合成 |
2021-08-17 | |
Source Publication | ACS Catalysis |
Volume | 11Issue:17Pages:10902-10912 |
Abstract | 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. |
Keyword | heterogeneous catalysis oxidative amination amide porous carbon nitrogen-doped carbon phosphorus-doped carbon metal-free carbon catalyst |
DOI | 10.1021/acscatal.1c02264 |
Indexed By | SCI |
If | 13.084 |
Language | 英语 |
compositor | 第一作者单位 |
Citation statistics | |
Document Type | 期刊论文 |
Identifier | http://ir.licp.cn/handle/362003/27684 |
Collection | 羰基合成与选择氧化国家重点实验室(OSSO) |
Corresponding Author | Li Fuwei |
Affiliation | 1.State Key Laboratory for Oxo Synthesis and Selective Oxidation, Lanzhou Institute of Chemical Physics, Chinese Academy of Sciences, Lanzhou 730000, China 2.These authors contributed equally: Long Xiangdong, Wang Jia. |
Recommended Citation GB/T 7714 | Long Xiangdong,Wang Jia,Gao Guang,等. 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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Direct Oxidative Ami(4680KB) | 期刊论文 | 作者接受稿 | 开放获取 | CC BY-NC-SA | View Application Full Text |
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