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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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    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. Tao Zhang & Qitong Ye & Zengyu Han & Qingyi Liu & Yipu Liu & Dongshuang Wu & Hong Jin Fan, 2024. "Biaxial strain induced OH engineer for accelerating alkaline hydrogen evolution," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    3. 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.
    4. 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.
    5. 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.
    6. Zamljen, Aleksandra & Lavrič, Žan & Prašnikar, Anže & Teržan, Janvit & Grilc, Miha & Meden, Anton & Likozar, Blaž, 2024. "Understanding platinum-based H2 adsorption/ desorption kinetics during catalytic hydrogenation or hydrogen storage-related reactions," Renewable Energy, Elsevier, vol. 226(C).
    7. Feng Wu & Xiaokang Liu & Shiqi Wang & Longfei Hu & Sebastian Kunze & Zhenggang Xue & Zehao Shen & Yaxiong Yang & Xinqiang Wang & Minghui Fan & Hongge Pan & Xiaoping Gao & Tao Yao & Yuen Wu, 2024. "Identification of K+-determined reaction pathway for facilitated kinetics of CO2 electroreduction," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    8. 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.
    9. 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.
    10. Longsheng Cao & Fernando A. Soto & Dan Li & Tao Deng & Enyuan Hu & Xiner Lu & David A. Cullen & Nico Eidson & Xiao-Qing Yang & Kai He & Perla B. Balbuena & Chunsheng Wang, 2024. "Pd-Ru pair on Pt surface for promoting hydrogen oxidation and evolution in alkaline media," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    11. Jinjie Fang & Haiyong Wang & Qian Dang & Hao Wang & Xingdong Wang & Jiajing Pei & Zhiyuan Xu & Chengjin Chen & Wei Zhu & Hui Li & Yushan Yan & Zhongbin Zhuang, 2024. "Atomically dispersed Iridium on Mo2C as an efficient and stable alkaline hydrogen oxidation reaction catalyst," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
    12. Quanguo Zhang & Youzhou Jiao & Chao He & Roger Ruan & Jianjun Hu & Jingzheng Ren & Sara Toniolo & Danping Jiang & Chaoyang Lu & Yameng Li & Yi Man & Huan Zhang & Zhiping Zhang & Chenxi Xia & Yi Wang &, 2024. "Biological fermentation pilot-scale systems and evaluation for commercial viability towards sustainable biohydrogen production," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
    13. 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.
    14. Linjie Zhang & Haihui Hu & Chen Sun & Dongdong Xiao & Hsiao-Tsu Wang & Yi Xiao & Shuwen Zhao & Kuan Hung Chen & Wei-Xuan Lin & Yu-Cheng Shao & Xiuyun Wang & Chih-Wen Pao & Lili Han, 2024. "Bimetallic nanoalloys planted on super-hydrophilic carbon nanocages featuring tip-intensified hydrogen evolution electrocatalysis," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
    15. 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.
    16. 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.
    17. 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.
    18. 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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