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In-situ spectroscopic observation of dynamic-coupling oxygen on atomically dispersed iridium electrocatalyst for acidic water oxidation

Author

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  • Hui Su

    (National Synchrotron Radiation Laboratory, University of Science and Technology of China)

  • Wanlin Zhou

    (National Synchrotron Radiation Laboratory, University of Science and Technology of China)

  • Wu Zhou

    (School of Chemistry and Chemical Engineering, Key Laboratory for Green Processing of Chemical Engineering of Xinjiang Bingtuan, Shihezi University)

  • Yuanli Li

    (National Synchrotron Radiation Laboratory, University of Science and Technology of China)

  • Lirong Zheng

    (Beijing Synchrotron Radiation Facility, Institute of High Energy Physics, Chinese Academy of Sciences)

  • Hui Zhang

    (National Synchrotron Radiation Laboratory, University of Science and Technology of China)

  • Meihuan Liu

    (National Synchrotron Radiation Laboratory, University of Science and Technology of China)

  • Xiuxiu Zhang

    (National Synchrotron Radiation Laboratory, University of Science and Technology of China)

  • Xuan Sun

    (National Synchrotron Radiation Laboratory, University of Science and Technology of China)

  • Yanzhi Xu

    (National Synchrotron Radiation Laboratory, University of Science and Technology of China)

  • Fengchun Hu

    (National Synchrotron Radiation Laboratory, University of Science and Technology of China)

  • Jing Zhang

    (Beijing Synchrotron Radiation Facility, Institute of High Energy Physics, Chinese Academy of Sciences)

  • Tiandou Hu

    (Beijing Synchrotron Radiation Facility, Institute of High Energy Physics, Chinese Academy of Sciences)

  • Qinghua Liu

    (National Synchrotron Radiation Laboratory, University of Science and Technology of China)

  • Shiqiang Wei

    (National Synchrotron Radiation Laboratory, University of Science and Technology of China)

Abstract

Uncovering the dynamics of active sites in the working conditions is crucial to realizing increased activity, enhanced stability and reduced cost of oxygen evolution reaction (OER) electrocatalysts in proton exchange membrane electrolytes. Herein, we identify at the atomic level potential-driven dynamic-coupling oxygen on atomically dispersed hetero-nitrogen-configured Ir sites (AD-HN-Ir) in the OER working conditions to successfully provide the atomically dispersed Ir electrocatalyst with ultrahigh electrochemical acidic OER activity. Using in-situ synchrotron radiation infrared and X-ray absorption spectroscopies, we directly observe that one oxygen atom is formed at the Ir active site with an O-hetero-Ir-N4 structure as a more electrophilic active centre in the experiment, which effectively promotes the generation of key *OOH intermediates under working potentials; this process is favourable for the dissociation of H2O over Ir active sites and resistance to over-oxidation and dissolution of the active sites. The optimal AD-HN-Ir electrocatalyst delivers a large mass activity of 2860 A gmetal−1 and a large turnover frequency of 5110 h−1 at a low overpotential of 216 mV (10 mA cm−2), 480–510 times larger than those of the commercial IrO2. More importantly, the AD-HN-Ir electrocatalyst shows no evident deactivation after continuous 100 h OER operation in an acidic medium.

Suggested Citation

  • Hui Su & Wanlin Zhou & Wu Zhou & Yuanli Li & Lirong Zheng & Hui Zhang & Meihuan Liu & Xiuxiu Zhang & Xuan Sun & Yanzhi Xu & Fengchun Hu & Jing Zhang & Tiandou Hu & Qinghua Liu & Shiqiang Wei, 2021. "In-situ spectroscopic observation of dynamic-coupling oxygen on atomically dispersed iridium electrocatalyst for acidic water oxidation," Nature Communications, Nature, vol. 12(1), pages 1-9, December.
    • Handle: RePEc:nat:natcom:v:12:y:2021:i:1:d:10.1038_s41467-021-26416-3
    DOI: 10.1038/s41467-021-26416-3
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    Cited by:

    1. Wanlin Zhou & Baojie Li & Xinyu Liu & Jingjing Jiang & Shuowen Bo & Chenyu Yang & Qizheng An & Yuhao Zhang & Mikhail A. Soldatov & Huijuan Wang & Shiqiang Wei & Qinghua Liu, 2024. "In situ tuning of platinum 5d valence states for four-electron oxygen reduction," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
    2. Hui Su & Chenyu Yang & Meihuan Liu & Xu Zhang & Wanlin Zhou & Yuhao Zhang & Kun Zheng & Shixun Lian & Qinghua Liu, 2024. "Tensile straining of iridium sites in manganese oxides for proton-exchange membrane water electrolysers," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    3. Cristina Hora & Florin Ciprian Dan & Nicolae Rancov & Gabriela Elena Badea & Calin Secui, 2022. "Main Trends and Research Directions in Hydrogen Generation Using Low Temperature Electrolysis: A Systematic Literature Review," Energies, MDPI, vol. 15(16), pages 1-21, August.
    4. Hongnan Jia & Na Yao & Yiming Jin & Liqing Wu & Juan Zhu & Wei Luo, 2024. "Stabilizing atomic Ru species in conjugated sp2 carbon-linked covalent organic framework for acidic water oxidation," Nature Communications, Nature, vol. 15(1), pages 1-13, December.
    5. Zhirong Zhang & Chuanyi Jia & Peiyu Ma & Chen Feng & Jin Yang & Junming Huang & Jiana Zheng & Ming Zuo & Mingkai Liu & Shiming Zhou & Jie Zeng, 2024. "Distance effect of single atoms on stability of cobalt oxide catalysts for acidic oxygen evolution," Nature Communications, Nature, vol. 15(1), pages 1-9, December.
    6. 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.
    7. Jiao Lan & Zengxi Wei & Ying-Rui Lu & DeChao Chen & Shuangliang Zhao & Ting-Shan Chan & Yongwen Tan, 2023. "Efficient electrosynthesis of formamide from carbon monoxide and nitrite on a Ru-dispersed Cu nanocluster catalyst," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    8. Dongpeng Zhang & Yanxiao Li & Pengfei Wang & Jinyong Qu & Yi Li & Sihui Zhan, 2023. "Dynamic active-site induced by host-guest interactions boost the Fenton-like reaction for organic wastewater treatment," Nature Communications, Nature, vol. 14(1), pages 1-9, December.
    9. Pengcheng Ye & Keqing Fang & Haiyan Wang & Yahao Wang & Hao Huang & Chenbin Mo & Jiqiang Ning & Yong Hu, 2024. "Lattice oxygen activation and local electric field enhancement by co-doping Fe and F in CoO nanoneedle arrays for industrial electrocatalytic water oxidation," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
    10. Meihuan Liu & Jing Zhang & Hui Su & Yaling Jiang & Wanlin Zhou & Chenyu Yang & Shuowen Bo & Jun Pan & Qinghua Liu, 2024. "In situ modulating coordination fields of single-atom cobalt catalyst for enhanced oxygen reduction reaction," Nature Communications, Nature, vol. 15(1), pages 1-10, December.

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