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Key role of chemistry versus bias in electrocatalytic oxygen evolution

Author

Listed:
  • Hong Nhan Nong

    (Technische Universität Berlin
    Max-Planck-Institute for Chemical Energy Conversion)

  • Lorenz J. Falling

    (Fritz-Haber-Institute of the Max-Planck-Society)

  • Arno Bergmann

    (Fritz-Haber-Institute of the Max-Planck-Society)

  • Malte Klingenhof

    (Technische Universität Berlin)

  • Hoang Phi Tran

    (Technische Universität Berlin)

  • Camillo Spöri

    (Technische Universität Berlin)

  • Rik Mom

    (Fritz-Haber-Institute of the Max-Planck-Society)

  • Janis Timoshenko

    (Fritz-Haber-Institute of the Max-Planck-Society)

  • Guido Zichittella

    (ETH Zurich)

  • Axel Knop-Gericke

    (Max-Planck-Institute for Chemical Energy Conversion
    Fritz-Haber-Institute of the Max-Planck-Society)

  • Simone Piccinin

    (Consiglio Nazionale delle Ricerche, CNR-IOM)

  • Javier Pérez-Ramírez

    (ETH Zurich)

  • Beatriz Roldan Cuenya

    (Fritz-Haber-Institute of the Max-Planck-Society)

  • Robert Schlögl

    (Max-Planck-Institute for Chemical Energy Conversion
    Fritz-Haber-Institute of the Max-Planck-Society)

  • Peter Strasser

    (Technische Universität Berlin)

  • Detre Teschner

    (Max-Planck-Institute for Chemical Energy Conversion
    Fritz-Haber-Institute of the Max-Planck-Society)

  • Travis E. Jones

    (Fritz-Haber-Institute of the Max-Planck-Society)

Abstract

The oxygen evolution reaction has an important role in many alternative-energy schemes because it supplies the protons and electrons required for converting renewable electricity into chemical fuels1–3. Electrocatalysts accelerate the reaction by facilitating the required electron transfer4, as well as the formation and rupture of chemical bonds5. This involvement in fundamentally different processes results in complex electrochemical kinetics that can be challenging to understand and control, and that typically depends exponentially on overpotential1,2,6,7. Such behaviour emerges when the applied bias drives the reaction in line with the phenomenological Butler–Volmer theory, which focuses on electron transfer8, enabling the use of Tafel analysis to gain mechanistic insight under quasi-equilibrium9–11 or steady-state assumptions12. However, the charging of catalyst surfaces under bias also affects bond formation and rupture13–15, the effect of which on the electrocatalytic rate is not accounted for by the phenomenological Tafel analysis8 and is often unknown. Here we report pulse voltammetry and operando X-ray absorption spectroscopy measurements on iridium oxide to show that the applied bias does not act directly on the reaction coordinate, but affects the electrocatalytically generated current through charge accumulation in the catalyst. We find that the activation free energy decreases linearly with the amount of oxidative charge stored, and show that this relationship underlies electrocatalytic performance and can be evaluated using measurement and computation. We anticipate that these findings and our methodology will help to better understand other electrocatalytic materials and design systems with improved performance.

Suggested Citation

  • Hong Nhan Nong & Lorenz J. Falling & Arno Bergmann & Malte Klingenhof & Hoang Phi Tran & Camillo Spöri & Rik Mom & Janis Timoshenko & Guido Zichittella & Axel Knop-Gericke & Simone Piccinin & Javier P, 2020. "Key role of chemistry versus bias in electrocatalytic oxygen evolution," Nature, Nature, vol. 587(7834), pages 408-413, November.
  • Handle: RePEc:nat:nature:v:587:y:2020:i:7834:d:10.1038_s41586-020-2908-2
    DOI: 10.1038/s41586-020-2908-2
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    Citations

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    Cited by:

    1. Zeyu Wang & William A. Goddard & Hai Xiao, 2023. "Potential-dependent transition of reaction mechanisms for oxygen evolution on layered double hydroxides," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    2. Shiyi Chen & Shishi Zhang & Lei Guo & Lun Pan & Chengxiang Shi & Xiangwen Zhang & Zhen-Feng Huang & Guidong Yang & Ji-Jun Zou, 2023. "Reconstructed Ir‒O‒Mo species with strong Brønsted acidity for acidic water oxidation," Nature Communications, Nature, vol. 14(1), pages 1-13, December.
    3. Sheng Zhao & Sung-Fu Hung & Liming Deng & Wen-Jing Zeng & Tian Xiao & Shaoxiong Li & Chun-Han Kuo & Han-Yi Chen & Feng Hu & Shengjie Peng, 2024. "Constructing regulable supports via non-stoichiometric engineering to stabilize ruthenium nanoparticles for enhanced pH-universal water splitting," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
    4. Qian Dang & Haiping Lin & Zhenglong Fan & Lu Ma & Qi Shao & Yujin Ji & Fangfang Zheng & Shize Geng & Shi-Ze Yang & Ningning Kong & Wenxiang Zhu & Youyong Li & Fan Liao & Xiaoqing Huang & Mingwang Shao, 2021. "Iridium metallene oxide for acidic oxygen evolution catalysis," Nature Communications, Nature, vol. 12(1), pages 1-10, December.
    5. Inkyu Lee & Abhijith Surendran & Samantha Fleury & Ian Gimino & Alexander Curtiss & Cody Fell & Daniel J. Shiwarski & Omar Refy & Blaine Rothrock & Seonghan Jo & Tim Schwartzkopff & Abijeet Singh Meht, 2023. "Electrocatalytic on-site oxygenation for transplanted cell-based-therapies," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
    6. Wenxiang Zhu & Xiangcong Song & Fan Liao & Hui Huang & Qi Shao & Kun Feng & Yunjie Zhou & Mengjie Ma & Jie Wu & Hao Yang & Haiwei Yang & Meng Wang & Jie Shi & Jun Zhong & Tao Cheng & Mingwang Shao & Y, 2023. "Stable and oxidative charged Ru enhance the acidic oxygen evolution reaction activity in two-dimensional ruthenium-iridium oxide," Nature Communications, Nature, vol. 14(1), pages 1-12, December.
    7. Xin Zhang & Haoyin Zhong & Qi Zhang & Qihan Zhang & Chao Wu & Junchen Yu & Yifan Ma & Hang An & Hao Wang & Yiming Zou & Caozheng Diao & Jingsheng Chen & Zhi Gen Yu & Shibo Xi & Xiaopeng Wang & Junmin , 2024. "High-spin Co3+ in cobalt oxyhydroxide for efficient water oxidation," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
    8. Xiao Ren & Tianze Wu & Zizhao Gong & Lulu Pan & Jianling Meng & Haitao Yang & Freyja Bjork Dagbjartsdottir & Adrian Fisher & Hong-Jun Gao & Zhichuan J. Xu, 2023. "The origin of magnetization-caused increment in water oxidation," Nature Communications, Nature, vol. 14(1), pages 1-8, December.
    9. Yufei Zhao & Priyank V. Kumar & Xin Tan & Xinxin Lu & Xiaofeng Zhu & Junjie Jiang & Jian Pan & Shibo Xi & Hui Ying Yang & Zhipeng Ma & Tao Wan & Dewei Chu & Wenjie Jiang & Sean C. Smith & Rose Amal & , 2022. "Modulating Pt-O-Pt atomic clusters with isolated cobalt atoms for enhanced hydrogen evolution catalysis," Nature Communications, Nature, vol. 13(1), pages 1-11, December.
    10. Kui Fan & Wenfu Xie & Jinze Li & Yining Sun & Pengcheng Xu & Yang Tang & Zhenhua Li & Mingfei Shao, 2022. "Active hydrogen boosts electrochemical nitrate reduction to ammonia," Nature Communications, Nature, vol. 13(1), pages 1-13, December.
    11. Raj Pandya & Florian Dorchies & Davide Romanin & Jean-François Lemineur & Frédéric Kanoufi & Sylvain Gigan & Alex W. Chin & Hilton B. Aguiar & Alexis Grimaud, 2024. "Concurrent oxygen evolution reaction pathways revealed by high-speed compressive Raman imaging," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    12. Francisco Sarabia & Carlos Gomez Rodellar & Beatriz Roldan Cuenya & Sebastian Z. Oener, 2024. "Exploring dynamic solvation kinetics at electrocatalyst surfaces," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    13. Haoyin Zhong & Qi Zhang & Junchen Yu & Xin Zhang & Chao Wu & Hang An & Yifan Ma & Hao Wang & Jun Zhang & Yong-Wei Zhang & Caozheng Diao & Zhi Gen Yu & Shibo Xi & Xiaopeng Wang & Junmin Xue, 2023. "Key role of eg* band broadening in nickel-based oxyhydroxides on coupled oxygen evolution mechanism," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    14. Chia-Shuo Hsu & Jiali Wang & You-Chiuan Chu & Jui-Hsien Chen & Chia-Ying Chien & Kuo-Hsin Lin & Li Duan Tsai & Hsiao-Chien Chen & Yen-Fa Liao & Nozomu Hiraoka & Yuan-Chung Cheng & Hao Ming Chen, 2023. "Activating dynamic atomic-configuration for single-site electrocatalyst in electrochemical CO2 reduction," Nature Communications, Nature, vol. 14(1), pages 1-14, December.
    15. Benedikt Axel Brandes & Yogeshwaran Krishnan & Fabian Luca Buchauer & Heine Anton Hansen & Johan Hjelm, 2024. "Unifying the ORR and OER with surface oxygen and extracting their intrinsic activities on platinum," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
    16. Lingxi Zhou & Yangfan Shao & Fang Yin & Jia Li & Feiyu Kang & Ruitao Lv, 2023. "Stabilizing non-iridium active sites by non-stoichiometric oxide for acidic water oxidation at high current density," Nature Communications, Nature, vol. 14(1), pages 1-12, December.
    17. Zhaoping Shi & Ji Li & Yibo Wang & Shiwei Liu & Jianbing Zhu & Jiahao Yang & Xian Wang & Jing Ni & Zheng Jiang & Lijuan Zhang & Ying Wang & Changpeng Liu & Wei Xing & Junjie Ge, 2023. "Customized reaction route for ruthenium oxide towards stabilized water oxidation in high-performance PEM electrolyzers," Nature Communications, Nature, vol. 14(1), pages 1-14, December.
    18. Felix T. Haase & Arno Bergmann & Travis E. Jones & Janis Timoshenko & Antonia Herzog & Hyo Sang Jeon & Clara Rettenmaier & Beatriz Roldan Cuenya, 2022. "Size effects and active state formation of cobalt oxide nanoparticles during the oxygen evolution reaction," Nature Energy, Nature, vol. 7(8), pages 765-773, August.
    19. Yiming Zhu & Jiaao Wang & Toshinari Koketsu & Matthias Kroschel & Jin-Ming Chen & Su-Yang Hsu & Graeme Henkelman & Zhiwei Hu & Peter Strasser & Jiwei Ma, 2022. "Iridium single atoms incorporated in Co3O4 efficiently catalyze the oxygen evolution in acidic conditions," Nature Communications, Nature, vol. 13(1), pages 1-12, December.
    20. Carlos G. Rodellar & José M. Gisbert-Gonzalez & Francisco Sarabia & Beatriz Roldan Cuenya & Sebastian Z. Oener, 2024. "Ion solvation kinetics in bipolar membranes and at electrolyte–metal interfaces," Nature Energy, Nature, vol. 9(5), pages 548-558, May.
    21. Zhenhua Li & Xiaofan Li & Hua Zhou & Yan Xu & Si-Min Xu & Yue Ren & Yifan Yan & Jiangrong Yang & Kaiyue Ji & Li Li & Ming Xu & Mingfei Shao & Xianggui Kong & Xiaoming Sun & Haohong Duan, 2022. "Electrocatalytic synthesis of adipic acid coupled with H2 production enhanced by a ligand modification strategy," Nature Communications, Nature, vol. 13(1), pages 1-12, December.
    22. Yixin Hao & Sung-Fu Hung & Luqi Wang & Liming Deng & Wen-Jing Zeng & Chenchen Zhang & Zih-Yi Lin & Chun-Han Kuo & Ye Wang & Ying Zhang & Han-Yi Chen & Feng Hu & Linlin Li & Shengjie Peng, 2024. "Designing neighboring-site activation of single atom via tunnel ions for boosting acidic oxygen evolution," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    23. Yunzhou Wen & Cheng Liu & Rui Huang & Hui Zhang & Xiaobao Li & F. Pelayo García de Arquer & Zhi Liu & Youyong Li & Bo Zhang, 2022. "Introducing Brønsted acid sites to accelerate the bridging-oxygen-assisted deprotonation in acidic water oxidation," Nature Communications, Nature, vol. 13(1), pages 1-11, December.
    24. Earl Matthew Davis & Arno Bergmann & Chao Zhan & Helmut Kuhlenbeck & Beatriz Roldan Cuenya, 2023. "Comparative study of Co3O4(111), CoFe2O4(111), and Fe3O4(111) thin film electrocatalysts for the oxygen evolution reaction," Nature Communications, Nature, vol. 14(1), pages 1-10, December.

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