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The role of adsorbed hydroxide in hydrogen evolution reaction kinetics on modified platinum

Author

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  • Ian T. McCrum

    (Leiden University
    Clarkson University)

  • Marc T. M. Koper

    (Leiden University)

Abstract

The bifunctional mechanism that involves adsorbed hydroxide in the alkaline hydrogen oxidation and evolution reactions, important in hydrogen fuel cells and water electrolysers, is hotly debated. Hydroxide binding has been suggested to impact activity, but the exact role of adsorbed hydroxide in the reaction mechanism is unknown. Here, by selectively decorating steps on a Pt single crystal with other metal atoms, we show that the rate of alkaline hydrogen evolution exhibits a volcano-type relationship with the hydroxide binding strength. We find that Pt decorated with Ru at the step edge is 65 times more active for the hydrogen evolution reaction (HER) than is the bare Pt step. Simulations of electrochemical water dissociation show that the activation energy correlates with the OH* adsorption strength, even when the adsorbed hydroxide is not a product, which leads to a simulated volcano curve that matches the experimental curve. This work not only illustrates the alkaline HER mechanism but also provides a goal for catalyst design in targeting an optimum hydroxide binding strength to yield the highest rate for the alkaline HER. A three-dimensional (H and OH adsorbed species) HER activity volcano and the implications for hydrogen oxidation are discussed.

Suggested Citation

  • Ian T. McCrum & Marc T. M. Koper, 2020. "The role of adsorbed hydroxide in hydrogen evolution reaction kinetics on modified platinum," Nature Energy, Nature, vol. 5(11), pages 891-899, November.
    • Handle: RePEc:nat:natene:v:5:y:2020:i:11:d:10.1038_s41560-020-00710-8
    DOI: 10.1038/s41560-020-00710-8
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    8. Jiaxi Zhang & Longhai Zhang & Jiamin Liu & Chengzhi Zhong & Yuanhua Tu & Peng Li & Li Du & Shengli Chen & Zhiming Cui, 2022. "OH spectator at IrMo intermetallic narrowing activity gap between alkaline and acidic hydrogen evolution reaction," Nature Communications, Nature, vol. 13(1), pages 1-9, December.
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    11. Rubén Rizo & Julia Fernández-Vidal & Laurence J. Hardwick & Gary A. Attard & Francisco J. Vidal-Iglesias & Victor Climent & Enrique Herrero & Juan M. Feliu, 2022. "Investigating the presence of adsorbed species on Pt steps at low potentials," Nature Communications, Nature, vol. 13(1), pages 1-7, December.
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    14. Jon C. Wilson & Stavros Caratzoulas & Dionisios G. Vlachos & Yushan Yan, 2023. "Insights into solvent and surface charge effects on Volmer step kinetics on Pt (111)," Nature Communications, Nature, vol. 14(1), pages 1-9, December.
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