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<p>Electrochemical CO<sub>2</sub> reduction reaction (CO<sub>2</sub>RR) offers an attractive approach to produce chemicals and fuels, especially for the value-added multicarbon (C<sub>2+</sub>) products. However, due to the strong competition reactions of hydrogen evolution and mono-carbon production, precise modulation of reaction pathways at the molecular level is challenging. Here, we propose a dual-confinement effect of CO<sub>2</sub> reactant and *CO intermediate in CO<sub>2</sub>RR, induced by tuning the pore configuration of reconstructed covalent organic framework (RC-COF), which effectively improves C<sub>2+</sub> selectivity. Attributed to the dual-confinement effect, we achieved a maximum C<sub>2+</sub> selectivity of 67.0% at 500 mA cm<sup>−2</sup> over the COF modified Cu electrode, which maintains a high carbon products Faradaic efficiency over 90% across a board current density range (100–500 mA cm<sup>−2</sup>) in acidic electrolyte. Experimental and theoretical results prove that the highly crystalline RC-COF-1 with ordered micro-pores has advantages in modulating the adsorption and diffusion of reactants and intermediates. Our study provides deep insights into microenvironment modulation in CO<sub>2</sub>RR, and underscores the critical role of COF pore configuration for other heterogeneous catalysis reactions.</p>

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Dual-confinement of reconstructed covalent organic framework for enhanced CO2 electrolysis in acid

  • 期刊论文

  • 发表日期：

    2026年1月4日

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  • Xinyan Li,
  • Hongxu Gu,
  • Jipeng Xu,
  • Huan Wang,
  • Jiachen Wu,
  • Yining Xu,
  • Cheng Lian,
  • Qilin Cheng,
  • Weiwei Zhang,
  • Pengfei Liu,
  • Huagui Yang,
  • Wei-Hong Zhu

摘要

Electrochemical CO2 reduction reaction (CO2RR) offers an attractive approach to produce chemicals and fuels, especially for the value-added multicarbon (C2+) products. However, due to the strong competition reactions of hydrogen evolution and mono-carbon production, precise modulation of reaction pathways at the molecular level is challenging. Here, we propose a dual-confinement effect of CO2 reactant and *CO intermediate in CO2RR, induced by tuning the pore configuration of reconstructed covalent organic framework (RC-COF), which effectively improves C2+ selectivity. Attributed to the dual-confinement effect, we achieved a maximum C2+ selectivity of 67.0% at 500 mA cm−2 over the COF modified Cu electrode, which maintains a high carbon products Faradaic efficiency over 90% across a board current density range (100–500 mA cm−2) in acidic electrolyte. Experimental and theoretical results prove that the highly crystalline RC-COF-1 with ordered micro-pores has advantages in modulating the adsorption and diffusion of reactants and intermediates. Our study provides deep insights into microenvironment modulation in CO2RR, and underscores the critical role of COF pore configuration for other heterogeneous catalysis reactions.