Investigations Into Homogeneous Electrocatalytic H2 Production and NO2- Reduction Using a Variety of 3d Transition Metal Complexes

Abstract

Investigations into the homogeneous electrocatalytic capabilities and functionality of several 3d transition metal complexes for the generation of hydrogen and ammonia are presented herein. This research utilizes electrochemical, spectroscopic, and computational simulation techniques to probe the redox activity of organometallic complexes, identifying the active catalyst species and evaluating their catalytic capability. Co, Ni, and Fe are the selected metal centers used in each of the multidentate ligand systems. Non-innocent ligand contributions have been explored for each complex, uncovering a spectrum of participation within the catalytic mechanism across the catalogue of complexes, ranging from inert to intrinsically involved. Overall, this work aims to identify complexes capable of catalytic reduction reactions, evaluate their selectivity and kinetics, and elucidate details of their catalytic mechanisms.