| Summary: | Abstract Electrocatalytic hydrogen peroxide (H2O2) production via the two-electron oxygen reduction reaction is a promising alternative to the energy-intensive and high-pollution anthraquinone oxidation process. However, developing advanced electrocatalysts with high H2O2 yield, selectivity, and durability is still challenging, because of the limited quantity and easy passivation of active sites on typical metal-containing catalysts, especially for the state-of-the-art single-atom ones. To address this, we report a graphene/mesoporous carbon composite for high-rate and high-efficiency 2e− oxygen reduction catalysis. The coordination of pyrrolic-N sites -modulates the adsorption configuration of the *OOH species to provide a kinetically favorable pathway for H2O2 production. Consequently, the H2O2 yield approaches 30 mol g−1 h−1 with a Faradaic efficiency of 80% and excellent durability, yielding a high H2O2 concentration of 7.2 g L−1. This strategy of manipulating the adsorption configuration of reactants with multiple non-metal active sites provides a strategy to design efficient and durable metal-free electrocatalyst for 2e− oxygen reduction.
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