Discerning activity and inactivity in earth-abundant molecular oxygen evolution catalysts

Abstract

Most computational studies on the oxygen evolution reaction (OER) focus on systems which are known to catalyze this process experimentally. This work computationally examines a number of earth‐abundant metal (M=Mn, Fe, Co, Ni) complexes with tetradentate coordinating anionic ligands which, subject to the same experimental conditions, either evolve or do not evolve oxygen. We offer an account for the inactivity of catalysts and develop an effective thermodynamic descriptor to describe the activity of those catalysts that do evolve oxygen. Additionally, we describe how the functionalization of certain Fe OER catalysts can boost activity. Finally, to allow for the rapid evaluation of homogeneous OER catalysts within this family of complexes, high‐level heuristics to computationally screen these catalysts are detailed.