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A Planar, Conjugated N4-macrocyclic Cobalt Complex for Heterogeneous Electrocatalytic CO2 Reduction with High Activity.

Metal complexes have been widely investigated as promising electrocatalysts for CO 2 reduction. Most of the current research efforts mainly focus on ligands based on pyrrole subunits and the reported activities are still far from satisfactory. A novel planar and conjugated N4-macrocyclic cobalt complex (Co(II)CPY) derived from phenanthroline subunits is prepared herein, which delivers high activity for heterogeneous CO 2 electrocatalysis to CO in an aqueous medium and outperforms most of the metal complexes reported so far. At a molar loading of 5.93×10 -8 mol cm -2 , it exhibits a Faradaic efficiency of 96% and a turnover frequency of 9.59 s -1 towards CO at -0.70 V vs . RHE. The unraveling of electronic structural features suggests a synergistic effect from ligand to cobalt in Co(II)CPY plays a critical role in boosting its activity. As a result, the free energy difference for the formation of *COOH is lower than that on cobalt porphyrin, leading to enhanced CO production.