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

Junqi Song, Zhiqiang Zhang, Weiping Li, Chunli Liu, Guodong Feng, Yaqiong Su, Kai Xi (), Hong Yi (), Changhai Yi and Lan Peng ()
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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

Nature Communications, 2025, vol. 16, issue 1, 1-11

Abstract: 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.

Date: 2025
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DOI: 10.1038/s41467-025-64901-1

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