Enabling Direct H2O2 Production in Acidic Media through Rational Design of Transition Metal Single Atom Catalyst

By Jiajian Gao, H. Yang, Xiang Huang, Sung-Fu Hung, Weizheng Cai, Chunmiao Jia, S. Miao, Hao Ming Chen, Xiaofeng Yang, Yanqiang Huang and 2 more. Chem, 2020

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Summary 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.

Subfields: Materials Chemistry, Renewable Energy, Sustainability and the Environment

View Paper: https://www.semanticscholar.org/paper/261e589d7849458903a5d2f94912be52d1df620c