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Issue 7, 2019
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Understanding the high activity of mildly reduced graphene oxide electrocatalysts in oxygen reduction to hydrogen peroxide

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Abstract

The direct electrochemical synthesis of hydrogen peroxide (H2O2) would provide an attractive alternative to the traditional anthraquinone oxidation process for continuous on-site applications. Its industrial viability depends greatly on developing cost-effective catalysts with high activity and selectivity. Recent experiments have demonstrated that mildly reduced graphene oxide (mrGO) electrocatalysts exhibit highly selective and stable H2O2 formation activity [e.g., H. W. Kim, M. B. Ross, N. Kornienko, L. Zhang, J. Guo, P. Yang and B. D. McCloskey, Nat. Catal., 2018, 1, 282–290]. However, the identification of active site structures for this catalytic process on mrGO is doubtful. Herein, by means of first-principles calculations, we examine the H2O2 formation activities of the active site structures proposed in experiments and find that their activities are actually very low. Then, we systematically investigate the H2O2 formation activities of different oxygen functional group structures on mrGO based on experimental observations, and discover two types of oxygen functional group structures (2EP and 1ET + 1EP) that have comparable or even lower overpotentials (<0.10 V) for H2O2 formation compared with the state-of-the-art PtHg4 electrocatalyst. Our theoretical results reveal that the graphene edge and the synergetic effects between different oxygen functional groups are essential for the superior performance of mrGO for H2O2 production. This work not only provides a feasible explanation of the cause of high H2O2 formation activity of mrGO but also offers a guide for the design, synthesis, and mechanistic investigation of advanced carbon-based electrocatalysts for effective H2O2 production.

Graphical abstract: Understanding the high activity of mildly reduced graphene oxide electrocatalysts in oxygen reduction to hydrogen peroxide

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Publication details

The article was received on 14 Jan 2019, accepted on 26 Apr 2019 and first published on 10 May 2019


Article type: Communication
DOI: 10.1039/C9MH00066F
Mater. Horiz., 2019,6, 1409-1415

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    Understanding the high activity of mildly reduced graphene oxide electrocatalysts in oxygen reduction to hydrogen peroxide

    X. Tan, H. A. Tahini and S. C. Smith, Mater. Horiz., 2019, 6, 1409
    DOI: 10.1039/C9MH00066F

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