Activity–Selectivity Trends in the Electrochemical Production of Hydrogen Peroxide over Single-Site Metal–Nitrogen–Carbon Catalysts

Nitrogen-doped carbon materials featuring atomically dispersed metal cations (M-N-C) are an emerging family of materials with potential applications for electrocatalysis. The electrocatalytic activity of M-N-C materials toward four-electron oxygen reduction reaction (ORR) to H2O is a mainstream line of research for replacing platinum-group-metal based catalysts at the cathode of fuel cells. However, fundamental and practical aspects of their electrocatalytic activity toward two-electron ORR to H2O2, a future green “dream” process for chemical industry, remained poorly understood. Here we combined computational and experimental efforts to uncover the trends in electrochemical H2O2 production over a series of M-N-C materials (M=Mn, Fe, Co, Ni, and Cu) exclusively comprising atomically dispersed M-Nx sites from molecular first principles to bench-scale electrolyzers operating at industrial cur-rent density. We investigated the effect of the nature of 3d-metal within a series of M-N-C catalysts on electrocata...