High-throughput design of metal-nonmetal integrated catalytic pairs on nitrogenated holey graphene for electrocatalytic hydrogen peroxide production.

Hydrogen peroxide (H2O2) production via the two-electron oxygen reduction reaction (2e- ORR) under ambient conditions offers a promising alternative to the industrial process, highlighting the need for stable and efficient catalysts. Inspired by the potential of integrative catalytic pairs (ICPs), we constructed a series of ICPs supported on nitrogenated holey graphene (C2N, a 2D holey carbon nitride framework with a C:N ratio of 2:1) by embedding metal and nonmetal atoms (ICPs/C2N). Among all candidates, Cu-B/C2N exhibited a record-low overpotential of 0.00 V, which originates from its unique electronic structure and exceptional stability, reflecting a strong synergistic effect between Cu and B in tuning OOH⁎ adsorption. Furthermore, machine learning based on the extreme gradient boosting regression model, combined with SHapley Additive exPlanations analysis, revealed that catalytic activity originates from the synergistic interplay between electronic modulation and geometric coordination at dual-metal sites. This work provides an efficient route to accelerate the discovery of high-performance ICP-based catalysts by combining theoretical calculations with machine learning insights.