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Asymmetric dinitrogen-coordinated nickel single-atomic sites for efficient CO2 electroreduction

Author

Listed:
  • Yuzhu Zhou

    (University of Science and Technology of China)

  • Quan Zhou

    (University of Science and Technology of China)

  • Hengjie Liu

    (University of Science and Technology of China)

  • Wenjie Xu

    (University of Science and Technology of China)

  • Zhouxin Wang

    (University of Science and Technology of China)

  • Sicong Qiao

    (University of Science and Technology of China)

  • Honghe Ding

    (University of Science and Technology of China)

  • Dongliang Chen

    (Chinese Academy of Sciences)

  • Junfa Zhu

    (University of Science and Technology of China)

  • Zeming Qi

    (University of Science and Technology of China)

  • Xiaojun Wu

    (University of Science and Technology of China)

  • Qun He

    (University of Science and Technology of China)

  • Li Song

    (University of Science and Technology of China)

Abstract

Developing highly efficient, selective and low-overpotential electrocatalysts for carbon dioxide (CO2) reduction is crucial. This study reports an efficient Ni single-atom catalyst coordinated with pyrrolic nitrogen and pyridinic nitrogen for CO2 reduction to carbon monoxide (CO). In flow cell experiments, the catalyst achieves a CO partial current density of 20.1 mA cmgeo−2 at −0.15 V vs. reversible hydrogen electrode (VRHE). It exhibits a high turnover frequency of over 274,000 site−1 h−1 at −1.0 VRHE and maintains high Faradaic efficiency of CO (FECO) exceeding 90% within −0.15 to −0.9 VRHE. Operando synchrotron-based infrared and X-ray absorption spectra, and theoretical calculations reveal that mono CO-adsorbed Ni single sites formed during electrochemical processes contribute to the balance between key intermediates formation and CO desorption, providing insights into the catalyst’s origin of catalytic activity. Overall, this work presents a Ni single-atom catalyst with good selectivity and activity for CO2 reduction while shedding light on its underlying mechanism.

Suggested Citation

  • Yuzhu Zhou & Quan Zhou & Hengjie Liu & Wenjie Xu & Zhouxin Wang & Sicong Qiao & Honghe Ding & Dongliang Chen & Junfa Zhu & Zeming Qi & Xiaojun Wu & Qun He & Li Song, 2023. "Asymmetric dinitrogen-coordinated nickel single-atomic sites for efficient CO2 electroreduction," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
  • Handle: RePEc:nat:natcom:v:14:y:2023:i:1:d:10.1038_s41467-023-39505-2
    DOI: 10.1038/s41467-023-39505-2
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    References listed on IDEAS

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    Cited by:

    1. Xiubei Yang & Qizheng An & Xuewen Li & Yubin Fu & Shuai Yang & Minghao Liu & Qing Xu & Gaofeng Zeng, 2024. "Charging modulation of the pyridine nitrogen of covalent organic frameworks for promoting oxygen reduction reaction," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
    2. Chao-Hai Gu & Song Wang & Ai-Yong Zhang & Chang Liu & Jun Jiang & Han-Qing Yu, 2024. "Tuning electronic structure of metal-free dual-site catalyst enables exclusive singlet oxygen production and in-situ utilization," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    3. Zhibo Yao & Hao Cheng & Yifei Xu & Xinyu Zhan & Song Hong & Xinyi Tan & Tai-Sing Wu & Pei Xiong & Yun-Liang Soo & Molly Meng-Jung Li & Leiduan Hao & Liang Xu & Alex W. Robertson & Bingjun Xu & Ming Ya, 2024. "Hydrogen radical-boosted electrocatalytic CO2 reduction using Ni-partnered heteroatomic pairs," Nature Communications, Nature, vol. 15(1), pages 1-15, December.

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