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Efficient reduction of CO 2  into useful carbon resources particularly CO is an essential reaction for developing alternate sources of fuels and for reducing the greenhouse effect of CO 2 . The binuclear Ni, Fe − containing carbon monoxide dehydrogenase (CODHs) efficiently catalyzes the reduction of CO 2  to CO. The location of Ni and Fe at proper positions allows their cooperation for CO 2  to CO conversion through a push−pull mechanism. Bio−inspired from CODHs, we used several cofacial porphyrin dimers with different substituents as suitable ligands for holding two Fe ions with suitable Fe−Fe separation distance to efficiently and selectively promote CO 2  to CO conversion with high turnover frequencies, TOFs. The substituents on the porphyrin rings greatly affect the catalysis process. By introducing electron-withdrawing/-donating groups, e.g. electron-withdrawing perfluorophenyl, at all meso positions of the porphyrin rings, the catalysis overpotential,  η  was minimized by ≈0.3 V compared to that obtained by introducing electron-donating mesityl groups. The Fe porphyrin dimers among reported catalysts are the most efficient ones for CO 2  to CO conversion. Control experiments indicate that the high performance of the current CO 2  to CO conversion catalysts is due to the presence of binuclear Fe centers at suitable Fe−Fe separation distance.

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Bio-inspired cofacial Fe porphyrin dimers for efficient electrocatalytic CO2 to CO conversion: Overpotential tuning by substituents at the porphyrin rings