Integrated Two‐in‐one Strategy for Efficient Neutral Hydrogen Peroxide Electrosynthesis via Phosphorous Doping in 2D Mesoporous Carbon Carriers

Herein, we demonstrate a two‐in‐one strategy for efficient neutral electrosynthesis of H2O2 via two‐electron oxygen reduction reaction (2e−ORR), achieved by synergistically fine‐modulating both the local microenvironment and electronic structure of indium (In) single atom (SA) sites. Through a series of finite elemental simulations and experimental analysis, we highlight the significant impact of phosphorous (P) doping on an optimized 2D mesoporous carbon carrier, which fosters a favorable microenvironment by improving the mass transfer and O2 enrichment, subsequently leading to an increased local pH levels. Consequently, an outstanding 2e−ORR performance is observed in neutral electrolytes, achieving over 95% selectivity for H2O2 across a broad voltage range of 0.1 to 0.5 V vs RHE. In a flow cell, the production rate of H2O2 exceeds 22.54 mol gcat‐1 h‐1 while maintaining high stability at industrial‐level current densities. These results are comparable to, if not better than, those achieved under alkaline conditions. Further analysis, both experimental and theoretical, indicates that the P dopant occupies the second coordination sphere of the In SA, which shows optimized OOH* binding strength for an enhanced 2e‐ ORR kinetic.