Concurrent oxygen reduction and water oxidation at high ionic strength for scalable electrosynthesis of hydrogen peroxide

Changmin Kim, Sung O Park, Sang Kyu Kwak, Zhenhai Xia, Guntae Kim () and Liming Dai ()
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Changmin Kim: University of New South Wales
Sung O Park: Ulsan National Institute of Science and Technology (UNIST)
Sang Kyu Kwak: Ulsan National Institute of Science and Technology (UNIST)
Zhenhai Xia: University of New South Wales
Guntae Kim: Chinese Academy of Sciences
Liming Dai: University of New South Wales

Nature Communications, 2023, vol. 14, issue 1, 1-11

Abstract: Abstract Electrosynthesis of hydrogen peroxide via selective two-electron transfer oxygen reduction or water oxidation reactions offers a cleaner, cost-effective alternative to anthraquinone processes. However, it remains a challenge to achieve high Faradaic efficiencies at elevated current densities. Herein, we report that oxygen-deficient Pr1.0Sr1.0Fe0.75Zn0.25O4-δ perovskite oxides rich of oxygen vacancies can favorably bind the reaction intermediates to facilitate selective and efficient two-electron transfer pathways. These oxides exhibited superior Faradic efficiencies (~99%) for oxygen reduction over a wide potential range (0.05 to 0.45 V versus reversible hydrogen electrode) and current densities surpassing 50 mA cm−2 under high ionic strengths. We further found that the oxides perform a high selectivity (~80%) for two-electron transfer water oxidation reaction at a low overpotential (0.39 V). Lastly, we devised a membrane-free electrolyser employing bifunctional electrocatalysts, achieving a record-high Faradaic efficiency of 163.0% at 2.10 V and 50 mA cm−2. This marks the first report of the concurrent oxygen reduction and water oxidation catalysed by efficient bifunctional oxides in a novel membrane-free electrolyser for scalable hydrogen peroxide electrosynthesis.

Date: 2023
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DOI: 10.1038/s41467-023-41397-1

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