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Abstract The efficient electrosynthesis of hydrogen peroxide (H 2 O 2 ) via two‐electron oxygen reduction reaction (2e − ORR) in neutral media is undoubtedly a practical route, but the limited comprehension of electrocatalysts has hindered the system advancement. Herein, we present the design of model catalysts comprising mesoporous carbon spheres‐supported Pd nanoparticles for H 2 O 2 electrosynthesis at near‐zero overpotential with approximately 95 % selectivity in a neutral electrolyte. Impressively, the optimized Pd/MCS‐8 electrocatalyst in a flow cell device achieves an exceptional H 2 O 2 yield of 15.77 mol g catalyst −1 h −1 , generating a neutral H 2 O 2 solution with an accumulated concentration of 6.43 wt %, a level sufficiently high for medical disinfection. Finite element simulation and experimental results suggest that mesoporous carbon carriers promote O 2 enrichment and localized pH elevation, establishing a favorable microenvironment for 2e − ORR in neutral media. Density functional theory calculations reveal that the robust interaction between Pd nanoparticles and the carbon carriers optimized the adsorption of OOH* at the carbon edge, ensuring high active 2e − process. These findings offer new insights into carbon‐loaded electrocatalysts for efficient 2e − ORR in neutral media, emphasizing the role of carrier engineering in constructing favorable microenvironments and synergizing active sites.
Jing et al. (Mon,) studied this question.