NBOH Site‐Activated Graphene Quantum Dots for Boosting Electrochemical Hydrogen Peroxide Production

Carbon materials are considered promising 2/4 e^- oxygen reduction reaction (ORR) electrocatalysts for synthesizing H₂ O₂ /H₂ O via regulating heteroatom dopants and functionalization. Here, various doped and functionalized graphene quantum dots (GQDs) are designed to reveal the crucial active sites of carbon materials for ORR to produce H₂ O₂ . Density functional theory (DFT) calculations predict that the edge structure involving edge N, B dopant pairs and further OH functionalization to the B (NBOH) is an active center for 2e^- ORR. To verify the above predication, GQDs with an enriched density of NBOH (NBO-GQDs) are designed and synthesized by the hydrothermal reaction of NH₂ edge-functionalized GQDs with H₃ BO₃ forming six-member heterocycle containing the NBOH structure. When dispersed on conductive carbon substrates, the NBO-GQDs show H₂ O₂ selectivity of over 90% at 0.7 -0.8 V versus reversible hydrogen electrode in the alkaline solution in a rotating ring-disk electrode setup. The selectivity retains 90% of the initial value after 12 h stability test. In a flow cell setup, the H₂ O₂ production rate is up to 709 mmol g_catalyst ^-1 h^-1 , superior to most reported carbon- and metal-based electrocatalysts. This work provides molecular insight into the design and formulation of highly efficient carbon-based catalysts for sustainable H₂ O₂ production.