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Critical role of hydrogen sorption kinetics in electrocatalytic CO2 reduction revealed by on-chip in situ transport investigations

Author

Listed:
  • Zhangyan Mu

    (Nanjing University)

  • Na Han

    (Soochow University
    Jiangsu Key Laboratory for Advanced Negative Carbon Technologies)

  • Dan Xu

    (Nanjing University)

  • Bailin Tian

    (Nanjing University)

  • Fangyuan Wang

    (Nanjing University)

  • Yiqi Wang

    (Nanjing University)

  • Yamei Sun

    (Nanjing University)

  • Cheng Liu

    (Nanjing University)

  • Panke Zhang

    (Nanjing University)

  • Xuejun Wu

    (Nanjing University)

  • Yanguang Li

    (Soochow University
    Jiangsu Key Laboratory for Advanced Negative Carbon Technologies)

  • Mengning Ding

    (Nanjing University)

Abstract

Precise understanding of interfacial metal−hydrogen interactions, especially under in operando conditions, is crucial to advancing the application of metal catalysts in clean energy technologies. To this end, while Pd-based catalysts are widely utilized for electrochemical hydrogen production and hydrogenation, the interaction of Pd with hydrogen during active electrochemical processes is complex, distinct from most other metals, and yet to be clarified. In this report, the hydrogen surface adsorption and sub-surface absorption (phase transition) features of Pd and its alloy nanocatalysts are identified and quantified under operando electrocatalytic conditions via on-chip electrical transport measurements, and the competitive relationship between electrochemical carbon dioxide reduction (CO2RR) and hydrogen sorption kinetics is investigated. Systematic dynamic and steady-state evaluations reveal the key impacts of local electrolyte environment (such as proton donors with different pKa) on the hydrogen sorption kinetics during CO2RR, which offer additional insights into the electrochemical interfaces and optimization of the catalytic systems.

Suggested Citation

  • Zhangyan Mu & Na Han & Dan Xu & Bailin Tian & Fangyuan Wang & Yiqi Wang & Yamei Sun & Cheng Liu & Panke Zhang & Xuejun Wu & Yanguang Li & Mengning Ding, 2022. "Critical role of hydrogen sorption kinetics in electrocatalytic CO2 reduction revealed by on-chip in situ transport investigations," Nature Communications, Nature, vol. 13(1), pages 1-12, December.
    • Handle: RePEc:nat:natcom:v:13:y:2022:i:1:d:10.1038_s41467-022-34685-9
    DOI: 10.1038/s41467-022-34685-9
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    References listed on IDEAS

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    1. Ji Hoon Lee & Shyam Kattel & Zhao Jiang & Zhenhua Xie & Siyu Yao & Brian M. Tackett & Wenqian Xu & Nebojsa S. Marinkovic & Jingguang G. Chen, 2019. "Tuning the activity and selectivity of electroreduction of CO2 to synthesis gas using bimetallic catalysts," Nature Communications, Nature, vol. 10(1), pages 1-8, December.
    2. Mengning Ding & Qiyuan He & Gongming Wang & Hung-Chieh Cheng & Yu Huang & Xiangfeng Duan, 2015. "An on-chip electrical transport spectroscopy approach for in situ monitoring electrochemical interfaces," Nature Communications, Nature, vol. 6(1), pages 1-9, November.
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    1. Hang Xia & Xiaoru Sang & Zhiwen Shu & Zude Shi & Zefen Li & Shasha Guo & Xiuyun An & Caitian Gao & Fucai Liu & Huigao Duan & Zheng Liu & Yongmin He, 2023. "The practice of reaction window in an electrocatalytic on-chip microcell," Nature Communications, Nature, vol. 14(1), pages 1-10, December.

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