Effective H2O2 Electrosynthesis Enabled by Carbonyl Sites on Wrinkled Carbon Surface

Electrosynthesis of hydrogen peroxide (eH 2 O 2 ) offers a facile and environmentally benign synthesis alternative through selective two-electron oxygen reduction reaction (2e – ORR). Carbon-based nonprecious electrocatalysts are promising for 2e – ORR, however, its efficiency is often limited by low intrinsic activity and limited accessibility of catalytic sites. Here, we present a family of carbonyl rich carbon spheres with surface wrinkle structure, which was engineered to boost the activity for 2e – ORR and to enlarge its electrochemical active surface area. As compared to common O-doped carbon spheres, our materials with controlled surface wrinkles delivered a 10-fold enhancement of accessible active surface area. Extensive catalytic tests together with characterizations indicate carbonyl moieties are the predominant active sites for O 2 activation. In 0.1 M KOH electrolyte, the catalyst delivered the H 2 O 2 selectivity of > 97.5% over a large potential range from 0-0.67 V vs . RHE, which resulted in a H 2 O 2 production rate of 385 mmol/(g·h) at 0 V vs. RHE. This study provides a useful surface structure fine modulation method for the development of heteroatom-doped carbon electrocatalysts for selective H 2 O 2 synthesis.