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Uncovering near-free platinum single-atom dynamics during electrochemical hydrogen evolution reaction

Author

Listed:
  • Shi Fang

    (University of Science and Technology of China)

  • Xiaorong Zhu

    (Nanjing Normal University)

  • Xiaokang Liu

    (University of Science and Technology of China)

  • Jian Gu

    (University of Science and Technology of China)

  • Wei Liu

    (University of Science and Technology of China)

  • Danhao Wang

    (University of Science and Technology of China)

  • Wei Zhang

    (University of Science and Technology of China)

  • Yue Lin

    (University of Science and Technology of China)

  • Junling Lu

    (University of Science and Technology of China)

  • Shiqiang Wei

    (University of Science and Technology of China)

  • Yafei Li

    (Nanjing Normal University)

  • Tao Yao

    (University of Science and Technology of China)

Abstract

Single-atom catalysts offering intriguing activity and selectivity are subject of intense investigation. Understanding the nature of single-atom active site and its dynamics under working state are crucial to improving their catalytic performances. Here, we identify at atomic level a general evolution of single atom into a near-free state under electrocatalytic hydrogen evolution condition, via operando synchrotron X-ray absorption spectroscopy. We uncover that the single Pt atom tends to dynamically release from the nitrogen-carbon substrate, with the geometric structure less coordinated to support and electronic property closer to zero valence, during the reaction. Theoretical simulations support that the Pt sites with weakened Pt–support interaction and more 5d density are the real active centers. The single-atom Pt catalyst exhibits very high hydrogen evolution activity with only 19 mV overpotential in 0.5 M H2SO4 and 46 mV in 1.0 M NaOH at 10 mA cm−2, and long-term durability in wide-pH electrolytes.

Suggested Citation

  • Shi Fang & Xiaorong Zhu & Xiaokang Liu & Jian Gu & Wei Liu & Danhao Wang & Wei Zhang & Yue Lin & Junling Lu & Shiqiang Wei & Yafei Li & Tao Yao, 2020. "Uncovering near-free platinum single-atom dynamics during electrochemical hydrogen evolution reaction," Nature Communications, Nature, vol. 11(1), pages 1-8, December.
    • Handle: RePEc:nat:natcom:v:11:y:2020:i:1:d:10.1038_s41467-020-14848-2
    DOI: 10.1038/s41467-020-14848-2
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    Cited by:

    1. Hao Tan & Bing Tang & Ying Lu & Qianqian Ji & Liyang Lv & Hengli Duan & Na Li & Yao Wang & Sihua Feng & Zhi Li & Chao Wang & Fengchun Hu & Zhihu Sun & Wensheng Yan, 2022. "Engineering a local acid-like environment in alkaline medium for efficient hydrogen evolution reaction," Nature Communications, Nature, vol. 13(1), pages 1-9, December.
    2. Zengyao Wang & Jiyi Chen & Erhong Song & Ning Wang & Juncai Dong & Xiang Zhang & Pulickel M. Ajayan & Wei Yao & Chenfeng Wang & Jianjun Liu & Jianfeng Shen & Mingxin Ye, 2021. "Manipulation on active electronic states of metastable phase β-NiMoO4 for large current density hydrogen evolution," Nature Communications, Nature, vol. 12(1), pages 1-10, December.
    3. Wanlin Zhou & Hui Su & Weiren Cheng & Yuanli Li & Jingjing Jiang & Meihuan Liu & Feifan Yu & Wei Wang & Shiqiang Wei & Qinghua Liu, 2022. "Regulating the scaling relationship for high catalytic kinetics and selectivity of the oxygen reduction reaction," Nature Communications, Nature, vol. 13(1), pages 1-10, December.
    4. 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.
    5. Ruiling Zhang & Yaozhou Li & Xuan Zhou & Ao Yu & Qi Huang & Tingting Xu & Longtao Zhu & Ping Peng & Shuyan Song & Luis Echegoyen & Fang-Fang Li, 2023. "Single-atomic platinum on fullerene C60 surfaces for accelerated alkaline hydrogen evolution," Nature Communications, Nature, vol. 14(1), pages 1-12, December.
    6. Xiaowei Shi & Chao Dai & Xin Wang & Jiayue Hu & Junying Zhang & Lingxia Zheng & Liang Mao & Huajun Zheng & Mingshan Zhu, 2022. "Protruding Pt single-sites on hexagonal ZnIn2S4 to accelerate photocatalytic hydrogen evolution," Nature Communications, Nature, vol. 13(1), pages 1-10, December.
    7. 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.
    8. Zhenglong Fan & Fan Liao & Yujin Ji & Yang Liu & Hui Huang & Dan Wang & Kui Yin & Haiwei Yang & Mengjie Ma & Wenxiang Zhu & Meng Wang & Zhenhui Kang & Youyong Li & Mingwang Shao & Zhiwei Hu & Qi Shao, 2022. "Coupling of nanocrystal hexagonal array and two-dimensional metastable substrate boosts H2-production," Nature Communications, Nature, vol. 13(1), pages 1-10, 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. 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.
    11. Junsic Cho & Taejung Lim & Haesol Kim & Ling Meng & Jinjong Kim & Seunghoon Lee & Jong Hoon Lee & Gwan Yeong Jung & Kug-Seung Lee & Francesc Viñes & Francesc Illas & Kai S. Exner & Sang Hoon Joo & Cha, 2023. "Importance of broken geometric symmetry of single-atom Pt sites for efficient electrocatalysis," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    12. Yanghang Pan & Xinzhu Wang & Weiyang Zhang & Lingyu Tang & Zhangyan Mu & Cheng Liu & Bailin Tian & Muchun Fei & Yamei Sun & Huanhuan Su & Libo Gao & Peng Wang & Xiangfeng Duan & Jing Ma & Mengning Din, 2022. "Boosting the performance of single-atom catalysts via external electric field polarization," Nature Communications, Nature, vol. 13(1), pages 1-12, December.

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