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Self-healing Cu single-atom catalyst for high-performance electrocatalytic CO2 methanation

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  • Wanyu Shen

    (University of Science and Technology of China
    University of Science and Technology of China
    University of Science and Technology of China)

  • Xiaoping Gao

    (Ningbo University of Technology)

  • Qichen Liu

    (University of Science and Technology of China)

  • Peng Li

    (University of Science and Technology of China)

  • Rui Huang

    (University of Science and Technology of China)

  • Yi Tan

    (University of Science and Technology of China)

  • Zihan Wang

    (University of Science and Technology of China)

  • Yilin Zhang

    (University of Science and Technology of China)

  • Fan Zhao

    (University of Science and Technology of China
    University of Science and Technology of China)

  • Xin Wang

    (University of Science and Technology of China)

  • Shiyu Ji

    (University of Science and Technology of China
    University of Science and Technology of China
    University of Science and Technology of China)

  • Xusheng Zheng

    (University of Science and Technology of China)

  • Yu Zhang

    (University of Science and Technology of China
    University of Science and Technology of China
    University of Science and Technology of China)

  • Yuen Wu

    (University of Science and Technology of China
    University of Science and Technology of China
    University of Science and Technology of China)

Abstract

To address the escalating challenge of atmospheric CO2 emissions, this study proposes a self-healing Cu single atom (SA) catalyst design. By partially cleaving Cu-N bonds via hydrogen evolution reaction (HER), coordinatively unsaturated Cu sites form and spontaneously bond with adjacent ZrO2 clusters which are strategically positioned near the Cu SA, creating a hybrid Cu-N/O structure with enhanced performance. In situ Raman and X-ray absorption fine structure (XAFS) measurements confirm the dynamic reconstruction of coordination environment from CuN4 to CuN1O2 under electrochemical conditions. The reconstructed CuN1O2 achieve observed performance for CO2-to-CH4 conversion, reaching a Faradaic efficiency of 87.06 ± 3.22% at −500 mA cm−2 and 80.21 ± 1.01% at −1000 mA cm−2, which are threefold and tenfold higher than those of pristine CuN4. Furthermore, a 25-h stability test with 500 mA cm−2 current density in a membrane electrode assembly (MEA) electrolyzer demonstrates minimal activity decay (

Suggested Citation

  • Wanyu Shen & Xiaoping Gao & Qichen Liu & Peng Li & Rui Huang & Yi Tan & Zihan Wang & Yilin Zhang & Fan Zhao & Xin Wang & Shiyu Ji & Xusheng Zheng & Yu Zhang & Yuen Wu, 2025. "Self-healing Cu single-atom catalyst for high-performance electrocatalytic CO2 methanation," Nature Communications, Nature, vol. 16(1), pages 1-12, December.
    • Handle: RePEc:nat:natcom:v:16:y:2025:i:1:d:10.1038_s41467-025-63274-9
    DOI: 10.1038/s41467-025-63274-9
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