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.

Highlights

  • Bridging homogeneous and heterogeneous catalysis is a long-term pursuit in the field of catalysis

  • Cu was found to be an active catalyst for catalytic hydrogenation of CO2 to methanol[45] and nitrogencontaining ligand was usually used to tuning the catalytic performance of active metals[30,33]

  • We report a facile methodology for integration of nanoand molecular catalysis via catalytic synthesis of nitrogen doped carbon layers on AlOx supported nano-Cu

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Summary

Introduction

Bridging homogeneous and heterogeneous catalysis is a long-term pursuit in the field of catalysis. We report a facile methodology for integration of nanoand molecular catalysis via catalytic synthesis of nitrogen doped carbon layers on AlOx supported nano-Cu. 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 DMF from dimethylamine and This result well agrees our hypothesis, i.e., N-doped carbon layer can be in situ synthesized on the heterogenous catalyst sample during the reaction.

Results
Conclusion

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