摘要
Electrochemical oxygen reduction is a promising approach for the sustainable decentralized production of H_(2)O_(2),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 H_(2)O_(2).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 H_(2)O_(2) 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.
基金
This work was financially supported by the Natural Sciences and Engineering Research Council of Canada(NSERC),through the Discovery Grant Program(No.RGPIN-2018-06725)
the Discovery Accelerator Supplement Grant program(No.RGPAS2018-522651)
by the New Frontiers in Research FundExploration program(No.NFRFE-2019-00488).