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Activating dynamic atomic-configuration for single-site electrocatalyst in electrochemical CO2 reduction

Author

Listed:
  • Chia-Shuo Hsu

    (National Taiwan University)

  • Jiali Wang

    (National Taiwan University)

  • You-Chiuan Chu

    (National Taiwan University)

  • Jui-Hsien Chen

    (National Taiwan University)

  • Chia-Ying Chien

    (National Taiwan University)

  • Kuo-Hsin Lin

    (Industrial Technology Research Institute)

  • Li Duan Tsai

    (Industrial Technology Research Institute)

  • Hsiao-Chien Chen

    (Chang Gung University)

  • Yen-Fa Liao

    (National Synchrotron Radiation Research Center)

  • Nozomu Hiraoka

    (Japan Synchrotron Radiation Research Institute)

  • Yuan-Chung Cheng

    (National Taiwan University)

  • Hao Ming Chen

    (National Taiwan University
    National Synchrotron Radiation Research Center
    Taipei Medical University)

Abstract

One challenge for realizing high-efficiency electrocatalysts for CO2 electroreduction is lacking in comprehensive understanding of potential-driven chemical state and dynamic atomic-configuration evolutions. Herein, by using a complementary combination of in situ/operando methods and employing copper single-atom electrocatalyst as a model system, we provide evidence on how the complex interplay among dynamic atomic-configuration, chemical state change and surface coulombic charging determines the resulting product profiles. We further demonstrate an informative indicator of atomic surface charge (φe) for evaluating the CO2RR performance, and validate potential-driven dynamic low-coordinated Cu centers for performing significantly high selectivity and activity toward CO product over the well-known four N-coordinated counterparts. It indicates that the structural reconstruction only involved the dynamic breaking of Cu–N bond is partially reversible, whereas Cu–Cu bond formation is clearly irreversible. For all single-atom electrocatalysts (Cu, Fe and Co), the φe value for efficient CO production has been revealed closely correlated with the configuration transformation to generate dynamic low-coordinated configuration. A universal explication can be concluded that the dynamic low-coordinated configuration is the active form to efficiently catalyze CO2-to-CO conversion.

Suggested Citation

  • 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.
  • Handle: RePEc:nat:natcom:v:14:y:2023:i:1:d:10.1038_s41467-023-40970-y
    DOI: 10.1038/s41467-023-40970-y
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    Cited by:

    1. Jiali Wang & Chia-Shuo Hsu & Tai-Sing Wu & Ting-Shan Chan & Nian-Tzu Suen & Jyh-Fu Lee & Hao Ming Chen, 2023. "In situ X-ray spectroscopies beyond conventional X-ray absorption spectroscopy on deciphering dynamic configuration of electrocatalysts," Nature Communications, Nature, vol. 14(1), pages 1-23, December.
    2. Kaihang Yue & Yanyang Qin & Honghao Huang & Zhuoran Lv & Mingzhi Cai & Yaqiong Su & Fuqiang Huang & Ya Yan, 2024. "Stabilized Cu0 -Cu1+ dual sites in a cyanamide framework for selective CO2 electroreduction to ethylene," Nature Communications, Nature, vol. 15(1), pages 1-12, December.

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