Computational Discovery of Active and Selective Metal‐Nitrogen‐Graphene Catalysts for Electrooxidation of Water to H2O2

A direct electrosynthesis of H2O2 from either O2 or H2O is an attractive strategy to replace the energy-intensive industrial anthraquinone process. Two-electron water oxidation reaction (2e-WOR) offers several advantages over oxygen reduction such as better mass transfer due absence gas-phase reactants. However, 2e-WOR a more challenging and less studied process with only handful metal oxides exhibiting reasonable activity/selectivity properties. Herein, we employ density-functional-theory calculations screen variety metal-nitrogen-graphene structures for 2e-WOR. As consequence scaling between adsorption energies intermediates, determine linear relation selectivities first second steps 2e-WOR, viz. that if selectivity toward adsorbed OH improved, then at subsequent step decreased. We also find activity are linearly scaled in way higher (i.e., lower overpotential) leads formation step. Based on obtained results chemistries, e.g., containing NiNx−C moieties, predicted rival best-performing ZnO CaSnO3 terms combination their characteristics