Metal‐Free Boron‐Rich Borocarbonitride Catalysts for High‐Efficient Oxygen Reduction to Produce Hydrogen Peroxide†

Hydrogen peroxide (H2O2) is one of major chemical products in industrial production and daily life. The electrochemical method of two-electron oxygen reduction reaction (ORR) to synthesize H2O2 is a promising method. Carbon-based materials are considered to be ideal catalysts for H2O2 production by ORR because of its low price and good conductivity, but H2O2 selectivity of catalysts is still unsatisfactory due to the unreasonable electronic structure. Heteroatom doping is considered to be an effective method to adjust the electronic structure of electrocatalysts. Here, we report B, N co-doped graphite named borocarbonitride (BCN) materials with different atomic content as significant ORR catalysts. The relationship between the electronic structure of BCN catalysts and H2O2 selectivity was discovered. Specially, the born-rich BCN electrocatalyst with optimal doping amount of B and N not only exhibits excellent H2O2 selectivity of 71.7 % at the applied potential of 0.4 V in alkaline solution, but also shows good electrochemical stability. The excellent H2O2 selectivity of the BCN catalyst may be attributed to high content of B-C bonds and excellent ion mobility in electrolyte. This work not only provides a meaningful reference for designing the electronic structure of BCN catalysts to promote electrocatalytic H2O2 production, but also broadens the application of high efficient and stable metal-free electrocatalysts in the field of two-electron ORR.