How Metal Nuclearity Impacts Electrocatalytic H2 Production in Thiocarbohydrazone-Based Complexes

Thiocarbohydrazone-based catalysts feature ligands that are potentially electrochemically active. From the synthesis point of view, these can be easily tailored, opening multiple strategies for optimization, such as using different substituent groups or metal substitution. In this work, we show possibility a new strategy, involving nuclearity system, meaning number centers. We report and characterization trinuclear nickel-thiocarbohydrazone complex displaying an improved turnover rate compared with its mononuclear counterpart. use DFT calculations to mechanism involved is metal-centered, unlike metal-assisted ligand-centered found in complex. Finally, two possible mechanisms assigned catalyst, both initial double reduction system.