NBOH Site‐Activated Graphene Quantum Dots for Boosting Electrochemical Hydrogen Peroxide Production

Abstract Carbon materials are considered promising 2/4 e − oxygen reduction reaction (ORR) electrocatalysts for synthesizing H 2 O 2 /H 2 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 H 2 O 2 . 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 NH 2 edge‐functionalized GQDs with H 3 BO 3 forming six‐member heterocycle containing the NBOH structure. When dispersed on conductive carbon substrates, the NBO‐GQDs show H 2 O 2 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 H 2 O 2 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 H 2 O 2 production.