Abstract

Molecular electrocatalysis for carbon dioxide reduction reaction (CO2RR) based on metal porphyrins have reemerged as the artificial carbon cycle route to the global environment and climate crisis. But the misestimated electrocatalytic performance limited their practical applications. By molecular interfacial engineering, we studied comparatively the electrocatalytic performances of cobalt porphyrin (CoTPP), octathiophene grafted CoTPP (CoTDThPP) and polymerized CoTDThPP (P-CoTDThPP). Since their redox potentials were tuned successfully, the electroactive CoN4-centers amount were evaluated by well-defined cyclic voltammetry. Although the intrinsic electroactivity and selectivity between the three CoTPP assemblies were a little different, the current density and durability were promoted dramatically in the order P-CoTDThPP >> CoTDThPP > CoTPP, demonstrating the significance of molecular interfacial engineering on CO2RR system in improving the utilization rate of the CoN4 centers.

References

1. Ji, W.; Wang, T.-X.; Ding, X.; Lei, S.; Han, B.-H. Coord. Chem. Rev. 2021, 439.
2. Francke, R.; Schille, B.; Roemelt, M. Chem. Rev. 2018, 118, 4631-4701.