Journal
CHEM
Volume 6, Issue 3, Pages 658-674Publisher
CELL PRESS
DOI: 10.1016/j.chempr.2019.12.008
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Funding
- National Key R&D Program of China [2016YFA0202804]
- Singapore Ministry of Education Academic Research Fund (AcRF) [RG10/16, RG111/15, MOE2016-T2-2-004]
- Jiangsu Specially-Appointed Professor program
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The electrochemical oxygen reduction reaction in acidic media offers an attractive route for direct hydrogen peroxide (H2O2) generation and on-site applications, Unfortunately there is still a lack of cost-effective electrocatalysts with high catalytic performance. Here, we theoretically designed and experimentally demonstrated that a cobalt single-atom catalyst (Co SAC) anchored in nitrogen-doped graphene, with optimized adsorption energy of the *OOH intermediate, exhibited a high H2O2 production rate, which even slightly outperformed the state-of-the-art noble-metal-based electrocatalysts. The kinetic current of H2O2 production over Co SAC could reach 1 mA/cm(disk)(2) at 0.6 V versus reversible hydrogen electrode in 0.1 M HClO4 with H2O2 faraday efficiency > 90%, and these performance measures could be sustained for 10 h without decay. Further kinetic analysis and operando X-ray absorption study combined with density functional theory (DFT) calculation demonstrated that the nitrogen-coordinated single Co atom was the active site and the reaction was rate-limited by the first electron transfer step.
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