Active catalyst construction for CO<sub>2</sub> recycling via catalytic synthesis of N-doped carbon on supported Cu.

Wu, Yajuan; Wang, Tao; Wang, Hongli; Wang, Xinzhi; Dai, Xingchao; Shi, Feng · Nat Commun · 2019

basic_science · Level V

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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 CO<sub>2</sub>/H<sub>2</sub> via blocking reaction pathways of further catalytic hydrogenation of DMF to N(CH<sub>3</sub>)<sub>3</sub>. 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(CH<sub>3</sub>)<sub>3</sub>. Our primary results could promote merging of homogeneous catalysis and heterogeneous catalysis and CO<sub>2</sub> recycling.