https://scholars.lib.ntu.edu.tw/handle/123456789/575736
標題: | Enabling Direct H2O2 Production in Acidic Media through Rational Design of Transition Metal Single Atom Catalyst | 作者: | Gao J HAO MING CHEN et al. |
關鍵字: | catalyst design; electrocatalysis; hydrogen peroxide; oxygen reduction reaction; SDG7: Affordable and clean energy; SDG9: Industry, innovation, and infrastructure; single atom catalyst | 公開日期: | 2020 | 卷: | 6 | 期: | 3 | 起(迄)頁: | 658-674 | 來源出版物: | Chem | 摘要: | Hydrogen peroxide is a valuable chemical with extensive applications, but the current industrial production method is energy-intensive and generates substantial waste. The electrochemical oxygen reduction reaction in acidic media offers an attractive route for direct hydrogen peroxide generation and on-site applications. Unfortunately, there is still a lack of cost-effective electrocatalysts with high catalytic performance. Here, by combining theoretical calculations and experimental methods, we demonstrate that an atomically dispersed cobalt anchored in nitrogen-doped carbon can function as a highly active and selective electrocatalyst for direct hydrogen peroxide synthesis. This cobalt single-atom catalyst combines the advantages of both homogeneous catalysts of cobalt macrocycles (well-defined active sites) and heterogeneous metal-nitrogen-carbon catalysts (high catalytic performance) together, showing promising application in electrosynthesis device. ? 2019By combining theoretical and experimental methods, Gao et al. systematically studied the relationship between the structure of transition metal (Mn, Fe, Co, Ni, and Cu) single-atom catalyst anchored in nitrogen-doped graphene and the catalytic performance of hydrogen peroxide (H2O2) synthesis via electrochemical two-electron oxygen reduction reaction (ORR) (2e? ORR). The thus designed Co single-atom catalyst can function as a highly active and selective catalyst for H2O2 synthesis and even slightly outperforms state-of-the-art noble-metal-based electrocatalysts in acidic media. ? 2019The 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/cmdisk 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. ? 2019 |
URI: | https://www.scopus.com/inward/record.uri?eid=2-s2.0-85081030993&doi=10.1016%2fj.chempr.2019.12.008&partnerID=40&md5=00eccd37469bb173c598c902014112ec https://scholars.lib.ntu.edu.tw/handle/123456789/575736 |
ISSN: | 24519308 | DOI: | 10.1016/j.chempr.2019.12.008 |
顯示於: | 化學系 |
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