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Supercritical CO2-assisted rapid synthesis of covalent organic framework-based electrocatalyst for efficient two-electron oxygen reduction reaction

Author

Listed:
  • Junqi Song

    (Wuhan Textile University)

  • Zhiqiang Zhang

    (Wuhan University)

  • Weiping Li

    (Xi’an Jiaotong University)

  • Chunli Liu

    (Xi’an Jiaotong University)

  • Guodong Feng

    (Xi’an Jiaotong University)

  • Yaqiong Su

    (Xi’an Jiaotong University)

  • Kai Xi

    (Xi’an Jiaotong University)

  • Hong Yi

    (Wuhan University)

  • Changhai Yi

    (Wuhan Textile University)

  • Lan Peng

    (Wuhan Textile University)

Abstract

Covalent organic frameworks (COFs) hold significant promise as electrocatalysts, but their synthesis is typically constrained by prolonged reaction times (>72 h), high temperatures ( >120 °C), and the use of organic solvents. Conventional methods also involve multiple freeze-pump-thaw cycles, complicating scalability. Herein, we report a supercritical carbon dioxide (Sc-CO2)-assisted strategy for the rapid synthesis of COFs, enabling their direct in-situ growth on carbon substrates. This supercritical-solvothermal approach yields COF@CNT composites that exhibit effective electrocatalytic performance towards the two-electron oxygen reduction reaction (2e− ORR). The resulting catalysts achieve a H2O2 production rate of 94 mol gcat−1 h−1 and a Faradaic efficiency exceeding 95% at 800 mA cm−2. By reducing the consumption of organic solvents, shortening reaction durations, and circumventing high temperatures, this method provides a scalable and efficient route for COF synthesis. Overall, the Sc-CO2 strategy provides a promising platform for the rapid development of COF-based electrocatalysts, combining enhanced efficiency, scalability, and environmental compatibility.

Suggested Citation

  • Junqi Song & Zhiqiang Zhang & Weiping Li & Chunli Liu & Guodong Feng & Yaqiong Su & Kai Xi & Hong Yi & Changhai Yi & Lan Peng, 2025. "Supercritical CO2-assisted rapid synthesis of covalent organic framework-based electrocatalyst for efficient two-electron oxygen reduction reaction," Nature Communications, Nature, vol. 16(1), pages 1-11, December.
    • Handle: RePEc:nat:natcom:v:16:y:2025:i:1:d:10.1038_s41467-025-64901-1
    DOI: 10.1038/s41467-025-64901-1
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    References listed on IDEAS

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    1. Jiajun Zhao & Cehuang Fu & Ke Ye & Zheng Liang & Fangling Jiang & Shuiyun Shen & Xiaoran Zhao & Lu Ma & Zulipiya Shadike & Xiaoming Wang & Junliang Zhang & Kun Jiang, 2022. "Manipulating the oxygen reduction reaction pathway on Pt-coordinated motifs," Nature Communications, Nature, vol. 13(1), pages 1-10, December.
    2. Liu, Yaping & Wang, Ying & Huang, Diangui, 2019. "Supercritical CO2 Brayton cycle: A state-of-the-art review," Energy, Elsevier, vol. 189(C).
    3. Arthur G. Fink & Roxanna S. Delima & Alexandra R. Rousseau & Camden Hunt & Natalie E. LeSage & Aoxue Huang & Monika Stolar & Curtis P. Berlinguette, 2024. "Indirect H2O2 synthesis without H2," Nature Communications, Nature, vol. 15(1), pages 1-9, December.
    4. Xiao Zhou & Yuan Min & Changming Zhao & Cai Chen & Ming-Kun Ke & Shi-Lin Xu & Jie-Jie Chen & Yuen Wu & Han-Qing Yu, 2024. "Constructing sulfur and oxygen super-coordinated main-group electrocatalysts for selective and cumulative H2O2 production," Nature Communications, Nature, vol. 15(1), pages 1-13, December.
    5. 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.
    6. Lan Peng & Qianying Guo & Chaoyu Song & Samrat Ghosh & Huoshu Xu & Liqian Wang & Dongdong Hu & Lei Shi & Ling Zhao & Qiaowei Li & Tsuneaki Sakurai & Hugen Yan & Shu Seki & Yunqi Liu & Dacheng Wei, 2021. "Ultra-fast single-crystal polymerization of large-sized covalent organic frameworks," Nature Communications, Nature, vol. 12(1), pages 1-8, December.
    7. Peike Cao & Xie Quan & Xiaowa Nie & Kun Zhao & Yanming Liu & Shuo Chen & Hongtao Yu & Jingguang G. Chen, 2023. "Metal single-site catalyst design for electrocatalytic production of hydrogen peroxide at industrial-relevant currents," Nature Communications, Nature, vol. 14(1), pages 1-12, December.
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