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

Author

Listed:
  • 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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    Cited by:

    1. 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.
    2. 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.
    3. Xingdong Wang & Xuerui Liu & Jinjie Fang & Houpeng Wang & Xianwei Liu & Haiyong Wang & Chengjin Chen & Yongsheng Wang & Xuejiang Zhang & Wei Zhu & Zhongbin Zhuang, 2024. "Tuning the apparent hydrogen binding energy to achieve high-performance Ni-based hydrogen oxidation reaction catalyst," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    4. 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.
    5. Yong-Qing Yan & Ya Chen & Zhao Wang & Li-Hua Chen & Hao-Lin Tang & Bao-Lian Su, 2023. "Electrochemistry-assisted selective butadiene hydrogenation with water," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    6. Jiayi Chen & Mohammed Aliasgar & Fernando Buendia Zamudio & Tianyu Zhang & Yilin Zhao & Xu Lian & Lan Wen & Haozhou Yang & Wenping Sun & Sergey M. Kozlov & Wei Chen & Lei Wang, 2023. "Diversity of platinum-sites at platinum/fullerene interface accelerates alkaline hydrogen evolution," Nature Communications, Nature, vol. 14(1), pages 1-12, December.
    7. Ziqi Zhang & Zhe Zhang & Cailing Chen & Rui Wang & Minggang Xie & Sheng Wan & Ruige Zhang & Linchuan Cong & Haiyan Lu & Yu Han & Wei Xing & Zhan Shi & Shouhua Feng, 2024. "Single-atom platinum with asymmetric coordination environment on fully conjugated covalent organic framework for efficient electrocatalysis," Nature Communications, Nature, vol. 15(1), pages 1-13, December.
    8. Gaoxin Lin & Zhuang Zhang & Qiangjian Ju & Tong Wu & Carlo U. Segre & Wei Chen & Hongru Peng & Hui Zhang & Qiunan Liu & Zhi Liu & Yifan Zhang & Shuyi Kong & Yuanlv Mao & Wei Zhao & Kazu Suenaga & Fuqi, 2023. "Bottom-up evolution of perovskite clusters into high-activity rhodium nanoparticles toward alkaline hydrogen evolution," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    9. Tianyu Zhang & Jing Jin & Junmei Chen & Yingyan Fang & Xu Han & Jiayi Chen & Yaping Li & Yu Wang & Junfeng Liu & Lei Wang, 2022. "Pinpointing the axial ligand effect on platinum single-atom-catalyst towards efficient alkaline hydrogen evolution reaction," Nature Communications, Nature, vol. 13(1), pages 1-14, December.
    10. Pushkar G. Ghanekar & Siddharth Deshpande & Jeffrey Greeley, 2022. "Adsorbate chemical environment-based machine learning framework for heterogeneous catalysis," Nature Communications, Nature, vol. 13(1), pages 1-12, December.
    11. Yunqing Kang & Ovidiu Cretu & Jun Kikkawa & Koji Kimoto & Hiroki Nara & Asep Sugih Nugraha & Hiroki Kawamoto & Miharu Eguchi & Ting Liao & Ziqi Sun & Toru Asahi & Yusuke Yamauchi, 2023. "Mesoporous multimetallic nanospheres with exposed highly entropic alloy sites," Nature Communications, Nature, vol. 14(1), pages 1-12, December.

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