Chemically Engineering Multiple Active Sites in N, P, O-Tridoped Carbocatalyst: Unveiling Structure–Performance Relationship for Efficient Electrochemical Production of Hydrogen Peroxide

Electrocatalytic synthesis emerges as a promising approach for H2O2 production, yet simultaneously achieving high activity and selectivity remains a challenge. The breakthrough hinges on the development of efficient catalysts and a deep exploration of the structure–performance relationship. Herein, a novel N, P, and O-tridoped carbocatalyst is synthesized via triazine reaction using terephthalonitrile as the building block and phosphorus pentoxide as the functional reagent. This catalyst exhibits remarkable activity and selectivity for the electrocatalytic oxygen reduction reaction (ORR) two-electron pathway, achieving a kinetic current density of 60.65 mA cm–2 and a mass activity up to 59.0 A g–1. Furthermore, it demonstrates potential in the electrochemical synthesis of H2O2, with a production rate of 16.32 mg cm–2 h–1 and a Faraday efficiency (FE) of over 90% within a wide voltage range of 0.1–0.6 V. Combined with the theoretical calculations, this work provides a valuable insight for identifying key structural characters in the electrocatalytic ORR two-electron pathway.