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Origin of the Activity of Co–N–C Catalysts for Chemoselective Hydrogenation of Nitroarenes
ACS Catalysis ( IF 11.3 ) Pub Date : 2021-02-22 , DOI: 10.1021/acscatal.0c05479
Muhong Li 1 , Shanyong Chen 1 , Qike Jiang 2 , Qingliang Chen 1 , Xuan Wang 1 , Yong Yan 1 , Jian Liu 1 , Changchang Lv 1 , Weiping Ding 1 , Xuefeng Guo 1
Affiliation  

The production of functionalized anilines by chemoselective hydrogenation of nitroarenes occupies an important position in the chemical industries. Recently, cobalt and nitrogen codoped carbon (Co–N–C) catalysts have been reported to show outstanding catalytic performance in this process, whereas the nature of their active sites is still at the center of intense debate. In this paper, based on the well-controlled experiments on four types of typical Co–N–C materials derived from different methodologies, several unusual generalities in the hydrogenation of nitroarenes are clearly revealed, including protic-solvent dependence, antipoisoning, acid resistance, and reversible deactivation. Further investigations indicate that the single-atom species Co–Nx are the main active sites of the Co–N–C catalysts in this chemoselective hydrogenation process. The present work sheds light on the mechanism study on the metal–N–C catalysts and further contributes to the rational design of the high-performance single-atom catalysts.

中文翻译:

Co-NC催化硝基芳烃化学选择加氢活性的起源

通过硝基芳烃的化学选择性加氢生产功能化的苯胺在化学工业中占有重要地位。最近,据报道钴和氮共掺杂碳(Co–N–C)催化剂在此过程中表现出出色的催化性能,而其活性部位的性质仍处于激烈争论的中心。在本文中,基于通过不同方法获得的四种典型的Co-N-C材料的良好控制实验,清楚地揭示了硝基芳烃氢化中的几种不同寻常的一般性,包括对质子溶剂的依赖性,抗中毒性,耐酸性,和可逆的停用。进一步的研究表明,单原子物种Co–N x是该化学选择性加氢过程中Co–N–C催化剂的主要活性中心。目前的工作为金属-N-C催化剂的机理研究提供了启示,并进一步为高性能单原子催化剂的合理设计做出了贡献。
更新日期:2021-03-05
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