High-throughput screening and rational design to drive discovery in molecular water oxidation catalysis
Michael Craig, Max García‐Melchor
Abstract
The difficulty of the oxygen evolution reaction (OER) is a fundamental impediment to the sustainable production of hydrogen, in which molecular catalysts show the most impressive activity in terms of turnover frequency. Here, we interrogate 444 automatically generated molecular water oxidation catalysts composed of well-known ligand scaffolds and 6 different transition metals (Cr, Mn, Fe, Ru, Co, and Ni). These data confirm the method-independent universal scaling relationship for water oxidation catalysts, describe routes toward circumventing this relationship, and justify the ascendency of Ru catalysts for this reaction. Leveraging this information while applying catalyst design principles, we summarize experimental results, giving credence to our prediction of 9 earth-abundant molecular catalysts with theoretical overpotentials ranging from 200 to 400 mV as promising leads for experimental investigation. We also establish insights into spin-dependent scaling relations for key OER intermediates. Altogether, this work outlines the first steps toward enabling inverse design for molecular OER catalysts.