Research Article


2020, 13(11): 3082–3087


Controlling N-doping type in carbon to boost single-atom site Cu catalyzed transfer hydrogenation of quinoline

Jian Zhang1,§, Caiyan Zheng2,§, Maolin Zhang3, Yajun Qiu1, Qi Xu1, Weng-Chon Cheong4, Wenxing Chen5, Lirong Zheng6, Lin Gu7, Zhengpeng Hu2, Dingsheng Wang1 (✉), and Yadong Li1 (✉)

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1 Department of Chemistry, Tsinghua University, Beijing 100084, China
2 School of Physics, Nankai University, Tianjin 300071, China
3 KAUST Catalysis Center (KCC), King Abdullah University of Science and Technology, Thuwal 23955-6900, Saudi Arabia
4 Department of Physics and Chemistry, Faculty of Science and Technology, University of Macau, Taipa, Macau SAR, China
5 School of Materials Science and Engineering, Beijing Institute of Technology, Beijing 100081, China
6 Beijing Synchrotron Radiation Facility, Institute of High Energy Physics, Chinese Academy of Sciences, Beijing 100049, China
7 Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences, Beijing 100190, China
§ Jian Zhang and Caiyan Zheng contributed equally to this work.

Keywords: nitrogen-doping type, metal oxide, nitrogen-doped carbon, single-atom site catalyst, transfer hydrogenation
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Single-atom site (SA) catalysts on N-doped carbon (CN) materials exhibit prominent performance for their active sites being M-Nx. Due to the commonly random doping behaviors of N species in these CN, it is a tough issue to finely regulate their doping types and clarify their effect on the catalytic property of such catalysts. Herein, we report that the N-doping type in CN can be dominated as pyrrolic-N and pyridinic-N respectively through compounding with different metal oxides. It is found that the proportion of distinct doped N species in CN depends on the acidity and basicity of compounded metal oxide host. Owing to the coordination by pyrrolic-N, the SA Cu catalyst displays an enhanced activity (two-fold) for transfer hydrogenation of quinoline to access the valuable molecule tetrahydroquinoline with a good selectivity (99%) under mild conditions. The higher electron density of SA Cu species induced by the predominate pyrrolic-N coordination benefits the hydrogen transfer process and reduces the energy barrier of the hydrogenation pathway, which accounts for the improved catalytic effeciency.
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Controlling N-doping type in carbon to boost single-atom site Cu catalyzed transfer hydrogenation of quinoline. Nano Res. 2020, 13(11): 3082–3087

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