Active catalyst construction for CO2 recycling via catalytic synthesis of N-doped carbon on supported Cu.
Yajuan WuTao WangHongli WangXinzhi WangXingchao DaiFeng ShiPublished in: Nature communications (2019)
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.
Keyphrases
- visible light
- metal organic framework
- highly efficient
- crystal structure
- room temperature
- ionic liquid
- density functional theory
- quantum dots
- reduced graphene oxide
- molecular dynamics
- gene expression
- molecular docking
- single molecule
- aqueous solution
- molecular dynamics simulations
- genome wide
- dna methylation
- carbon dioxide
- high density