Facing the 21st-century energy challenge, hydrogen production as an alternative fuel by catalytic water splitting is a central theme in the field of renewable energy storage. Platinum possesses the best performances among catalysts able to reduce protons to hydrogen. However, due to its scarcity and its cost, efforts to find alternative non-noble transition metal catalysts have been the subject of intense research.1 A number of molecular catalysts based on Earth-abundant metals have been developed in recent years. Together with the introduction of proton relays in the second coordination sphere of the metal center, redox-active ligands can be exploited to promote or enhance catalytic activity. Transition metal complexes with thiosemicarbazone ligands have been studied for many years as these complexes present some interesting features (redox properties, nitrogen or sulfur atoms as potential proton relays) for hydrogen evolution. In that perspective, we have associated the electroactive thiosemicarbazone ligand with redox-active transition metals like nickel,1,4 palladium2, and cobalt.3 We have reported on the experimental and theoretical characterization of the complexes as well as their evaluation as electrocatalysts for proton reduction in an effort to rationalize the influence of the metal center on the catalytic performances.5

Hydrogen evolution reaction by transition metal complexes with redox-active ligands

ACS Spring 2022

The official archive and repository for all ACS Meetings & Expositions abstracts and select posters or presentations.