Understanding how to precisely control substrate delivery and product removal from the active site of molecular catalysts has been an emphasis of the Center for Molecular Electrocatalysis in the development of efficient electrocatalysts for energy storage reactions. We have focused on using pendant amines in the secondary coordination sphere of nickel complexes to relay protons to and from the metal center for H2 production and oxidation catalysis, similar to the [Fe-Fe]-hydrogenase active site. Efficient proton movement by the pendant amines in the PR2NR′2 ligands to the metal center can increase the observed turnover frequency for H2 production dramatically, to greater than 106 s-1. Previous work has established that the efficiency of these proton relays is highly dependent on the medium composition as well as the structural dynamics of the catalyst, which control the positioning of the pendant amine relative to the metal center. Current work focuses on using ligand modifications to reduce the overpotentials required for these catalysts while maintaining the efficient proton movement necessary for fast turnover frequencies.

Reducing overpotential and maintaining high rates in nickel electrocatalysts for H2 production

253rd National Meeting (2017)

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