Proceedings of MATSUS Spring 2024 Conference (MATSUS24)
DOI: https://doi.org/10.29363/nanoge.matsus.2024.038
Publication date: 18th December 2023
Heterogeneous molecular catalysts based on transition metal complexes supported on conductive substrate have received increasing attention for their potential application in electrocatalysis and electrosynthesis. In this talk I will report some exemplary work on tuning the electrocatalytic activity of such heterogeneous molecular catalysts. The heterogenization of molecular catalyst was first demonstrated by anchoring molecular Co2+ ions onto N/S/O doped graphene. The S dopant of graphene is found to be most effective in improving the intrinsic activity of the Co sites. In another demonstration based on Ni molecular catalyst, we found for the first time that the presence of Fe3+ ions in the solution could bond at the vicinity of the Ni sites, generating heterogeneous Ni-Fe dual sites anchored on doped graphene. These Ni-Fe sites exhibited drastically improved oxygen evolution activity. Using CO2 reduction on well-defined molecular catalysts as a probe, we also demonstrated the importance of axial ligand, relay molecule and microenvironment in improving interfacial electron transfer and subsequent electrocatalytic activity.
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