Journal
ACS CATALYSIS
Volume 13, Issue 8, Pages 5114-5121Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.3c00494
Keywords
electrochemical CO2 reduction; metal-supramolecular pair catalyst; copper complex; secondary coordination sphere; dynamic conformation adaption
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This paper reports the use of a copper-supramolecular pair as a crystalline molecular catalyst to promote the formation of multicarbon products. Experimental and theoretical studies reveal the collaboration of paired Cu sites in activating the CO2 substrate and facilitating the coupling of adsorbed CO species. Van der Waals interactions between the substrate and the secondary coordination sphere also play a crucial role in multicarbon product selectivity.
Electrochemical CO2 reduction (ECR) into value-added multicarbon products is a promising approach for a carbon neutral economy. Heterogeneous molecular catalysts consist of atomic-precise, controllable active sites with the potential to improve catalytic activity by ligand design and engineering, yet most reported molecular ECR catalysts do not exhibit multicarbon product selectivity. Herein, we report the use of a copper-supramolecular pair as a crystalline molecular catalyst to promote the formation of multicarbon products. A combination of experimental and theoretical studies reveal that the paired Cu sites work collaboratively to activate the CO2 substrate and facilitate the coupling of adsorbed CO species although they are not bonded or bridged directly. The van der Waals interactions between the substrate and the secondary coordination sphere also play a crucial role in multicarbon product selectivity.
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