ACS Catalysis
ACS Catalysis
5 years ago

Electrode-Ligand Interactions Dramatically Enhance CO2 Conversion to CO by the [Ni(cyclam)](PF6)2 Catalyst

Electrode-Ligand Interactions Dramatically Enhance CO2 Conversion to CO by the [Ni(cyclam)](PF6)2 Catalyst
Victor S. Batista, Almagul Zhanaidarova, Benjamin Rudshteyn, Yueshen Wu, Wendu Ding, Jesse D. Froehlich, Clifford P. Kubiak
Dramatic enhancement of electrochemical CO2 conversion to CO, catalyzed by [Ni(cyclam)](PF6)2 is observed on mercury/gold electrodes. We find that Hg provides favorable noncovalent dispersive interactions with the cyclam ligand. As a result, the Hg surface destabilizes the poisoned CO-bound form of the catalyst, leading to enhanced reaction kinetics. These findings are particularly relevant to the design of ligands that improve the electrocatalytic performance of transition-metal complexes on interaction with metallic surfaces under cell operating conditions.

Publisher URL: http://dx.doi.org/10.1021/acscatal.7b01109

DOI: 10.1021/acscatal.7b01109

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