Find in Library

Hydrogen peroxide (H₂O₂) is an important chemical with a diverse range of industrial applications in chemical synthesis and medical disinfection. The traditional anthraquinone oxidation process, with high energy consumption and complexity, is being replaced by cost-effective and environmentally friendly alternatives. In order to explore suitable catalysts for the electrocatalytic synthesis of H₂O₂, the stability of B,N-doped graphene loaded with various p-block metal (PM) single atoms (i.e., PM-N_xB_y: x and y represent the number of atoms of N and B, respectively) and the effects of different numbers and positions of B dopants in the second coordination shell on the catalytic performance were studied by density functional theory (DFT) calculations. The results show that Ga-N₄B₆ and Sb-N₄B₆ exhibit enhanced stability and 2e⁻ oxygen reduction reaction (ORR) activity and selectivity. Their thermodynamic overpotential η values are 0.01 V, 0.03 V for Ga-N₄B₆’s two configurations and 0.02 V, 0 V for Sb-N₄B₆’s two configurations. Electronic structure calculations indicate that the PM single atom adsorbs OOH* intermediates and transfers electrons into them, resulting in the activation of the O-O bond, which facilitates the subsequent hydrogenation reaction. In summary, Sb-N₄B₆ and Ga-N₄B₆ exhibit extraordinary 2e⁻ ORR performance, and their predicted activities are comparable to those of known outstanding catalysts (such as PtHg₄ alloy). We propose effective strategies on how to enhance the 2e⁻ ORR activities of carbon materials, elucidate the origin of the activity of potential catalysts, and provide insights for the design and development of electrocatalysts that can be used for H₂O₂ production.