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BC2O Active Sites in Closed-Pore B,O-Doped Graphene Enable Selective H2O2 Electrosynthesis
Gang Bai1, Liuyue Cao2, Liang Du3
1State Key Laboratory of Advanced Chemical Power Sources, School of Chemistry and Chemical Engineering, Chongqing University, Chongqing, 400044, China.
None:
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 gcat -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.
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