Active catalyst construction for CO2 recycling via catalytic synthesis of N-doped carbon on supported Cu

Yajuan Wu, Tao Wang, Hongli Wang, Xinzhi Wang, Xingchao Dai and Feng Shi ()
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Yajuan Wu: Lanzhou Institute of Chemical Physics, Chinese Academy of Sciences
Tao Wang: Stanford University
Hongli Wang: Lanzhou Institute of Chemical Physics, Chinese Academy of Sciences
Xinzhi Wang: Lanzhou Institute of Chemical Physics, Chinese Academy of Sciences
Xingchao Dai: Lanzhou Institute of Chemical Physics, Chinese Academy of Sciences
Feng Shi: Lanzhou Institute of Chemical Physics, Chinese Academy of Sciences

Nature Communications, 2019, vol. 10, issue 1, 1-7

Abstract: Abstract Bridging homogeneous and heterogeneous catalysis is a long-term pursuit in the field of catalysis. Herein, we report our results in integration of nano- and molecular catalysis via catalytic synthesis of nitrogen doped carbon layers on AlOx supported nano-Cu which can finely tune the catalytic performance of the supported copper catalyst. This synthetic catalytic material, which can be generated in situ by the reaction of CuAlOx and 1,10-Phen in the presence of hydrogen, could be used for controllable synthesis of N,N-dimethylformamide (DMF) from dimethylamine and CO2/H2 via blocking reaction pathways of further catalytic hydrogenation of DMF to N(CH3)3. Detailed characterizations and DFT calculations reveal that the presence of N-doped layered carbon on the surface of the nano-Cu particles results in higher activation energy barriers during the conversion of DMF to N(CH3)3. Our primary results could promote merging of homogeneous catalysis and heterogeneous catalysis and CO2 recycling.

Date: 2019
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DOI: 10.1038/s41467-019-10633-y

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