BC 2 O Active Sites in Closed‐Pore B,O‐Doped Graphene Enable Selective H 2 O 2 Electrosynthesis

Carbon-based electrocatalysts are promising candidates for the two-electron oxygen reduction reaction (2e^- ORR) to produce H₂O₂. However, their low activity and selectivity hinder effective application. Herein, a closed-pore boron and oxygen co-doped graphene (B, O-graphene) catalysts are reported via thermal annealing of graphene oxide and boric acid under tunable H₂ atmospheres. The optimized closed-pore B, O-graphene catalyst exhibits outstanding 2e^- ORR performance, featuring >90% H₂O₂ selectivity across a wide potential window (≥0.3 V vs Reversible Hydrogen Electrode (RHE)), a remarkable production rate of 154.7 ± 2.3 mmol g_cat ^-1 h^-1, and a Faradaic efficiency of ≈96% at 0.3 V versus RHE. Combined experimental and theoretical studies reveal that the BC₂O moieties in the closed-pore graphene lattice, serve as the active centers, enabling exceptional selectivity.