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Electrochemical oxygen reduction is a promising approach for the sustainable decentralized production of H2O2, but its viable commercialization is hindered by the insufficient development of efficient electrocatalysts. Here, we demonstrate a promising carbon-based catalyst, consisting of oxygen-rich hollow mesoporous carbon spheres (HMCSs), for selective oxygen reduction to H2O2. The as-prepared HMCS exhibits high onset potential (0.82 V) and half-wave potential (0.76 V), delivering a significant positive shift compared with its oxygen-scarce counterparts and commercial Vulcan carbon. Moreover, excellent H2O2 selectivity (above 95%) and electrochemical stability (7% attenuation after 10 h operation) make this material a state-of-the-art catalyst for electrochemical H2O2 production. The outstanding performance arises from a combination of several aspects, such as porous structure-facilitation of mass transport, large surface area, and proper distribution of oxygen-containing functional groups modification on the surface. Furthermore, the proposed oxygen reduction reaction (ORR) mechanism on HMCS surface reveals that –OH functional groups help promote the first electron transfer process while other oxygen modification facilitate the second electron transfer.
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