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Abstract <p>A three-membrane electrolyzer has been designed for carbon dioxide (CO<sub>2</sub>) electroreduction to carbon monoxide (CO) in an organic electrolyte, with sodium carbonate (Na<sub>2</sub>CO<sub>3</sub>) and chlorine (Cl<sub>2</sub>) generated as by-products. In order to improve the performance of the electrolyzer, a heterostructured Ag/Cu catalyst was synthesized by growing spherical assemblies of Ag/Cu nanoflowers on Cu foam (AgNFs@CF). Experimental results combined with density functional theory (DFT) calculations reveal that tailoring the electric double-layer structure of the catalyst modulates the local microenvironment and effectively suppresses the hydrogen evolution reaction in the organic medium. Moreover, the synergistic interaction at the curved and interlaced interface between the Cu support and the Ag layer facilitates charge separation, thereby increasing the electron density at Ag sites. As a result, AgNFs@CF delivered a high CO partial current density of 162.68 mA cm<sup>−2</sup> at −2.4 V (vs. SHE), with a Faradaic efficiency of 92.6%, maintaining stability under prolonged electrolysis. This work provides both theoretical and experimental insights into designing the microenvironment of the Ag/Cu catalyst for efficient and eco-friendly CO production, while offering an industrially feasible route for converting CO<sub>2</sub> into high-value products.</p> Graphical abstract <p></p> 摘要 (Chinese Abstract) <p>本文构建了一种三膜电解体系, 在有机电解质中将二氧化碳 (CO<sub>2</sub>) 电还原为一氧化碳 (CO) , 同时联产碳酸钠 (Na<sub>2</sub>CO<sub>3</sub>) 和氯气 (Cl<sub>2</sub>) 。为提升反应性能, 制备了异质结构Ag/Cu催化剂 (AgNFs@CF) , AgNFs@CF由Ag/Cu纳米花球自组装在铜泡沫上。实验结果结合密度泛函理论 (DFT) 计算表明, 通过调控Ag/Cu催化剂的局部微环境, 可有效抑制有机电解液中的析氢反应。此外, Cu与Ag之间弯曲交错的界面促进了电荷分离, 提升了Ag位点的电子密度。在长周期电解过程中, AgNFs@CF在−2.4 V(vs. SHE) 下实现了162.68 mA cm<sup>−2</sup>的CO分电流密度和92.6%的法拉第效率。本研究从理论与实验两方面揭示了Ag/Cu微环境调控对提高CO<sub>2</sub>电还原效率的关键作用, 提供了一条具有工业应用潜力的CO<sub>2</sub>资源化利用新路径。</p>

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Engineering the Ag/Cu microenvironment for efficient CO2 electroreduction to CO in a three-membrane electrolyzer producing Na2CO3 and Cl2 by-products

  • 期刊论文

  • 发表日期：

    2025年10月21日

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  • Shuai Wu,
  • Tian-You Chen,
  • Jiang-Feng Mou,
  • Xin-Bo Shi,
  • Feng-Xia Shen,
  • Shi-Peng Miao,
  • Feng Shi,
  • Jian-Xiong Liu,
  • Ting Jin,
  • Jin Shi

摘要

Abstract

A three-membrane electrolyzer has been designed for carbon dioxide (CO2) electroreduction to carbon monoxide (CO) in an organic electrolyte, with sodium carbonate (Na2CO3) and chlorine (Cl2) generated as by-products. In order to improve the performance of the electrolyzer, a heterostructured Ag/Cu catalyst was synthesized by growing spherical assemblies of Ag/Cu nanoflowers on Cu foam (AgNFs@CF). Experimental results combined with density functional theory (DFT) calculations reveal that tailoring the electric double-layer structure of the catalyst modulates the local microenvironment and effectively suppresses the hydrogen evolution reaction in the organic medium. Moreover, the synergistic interaction at the curved and interlaced interface between the Cu support and the Ag layer facilitates charge separation, thereby increasing the electron density at Ag sites. As a result, AgNFs@CF delivered a high CO partial current density of 162.68 mA cm−2 at −2.4 V (vs. SHE), with a Faradaic efficiency of 92.6%, maintaining stability under prolonged electrolysis. This work provides both theoretical and experimental insights into designing the microenvironment of the Ag/Cu catalyst for efficient and eco-friendly CO production, while offering an industrially feasible route for converting CO2 into high-value products.

Graphical abstract

摘要 (Chinese Abstract)

本文构建了一种三膜电解体系, 在有机电解质中将二氧化碳 (CO2) 电还原为一氧化碳 (CO) , 同时联产碳酸钠 (Na2CO3) 和氯气 (Cl2) 。为提升反应性能, 制备了异质结构Ag/Cu催化剂 (AgNFs@CF) , AgNFs@CF由Ag/Cu纳米花球自组装在铜泡沫上。实验结果结合密度泛函理论 (DFT) 计算表明, 通过调控Ag/Cu催化剂的局部微环境, 可有效抑制有机电解液中的析氢反应。此外, Cu与Ag之间弯曲交错的界面促进了电荷分离, 提升了Ag位点的电子密度。在长周期电解过程中, AgNFs@CF在−2.4 V(vs. SHE) 下实现了162.68 mA cm−2的CO分电流密度和92.6%的法拉第效率。本研究从理论与实验两方面揭示了Ag/Cu微环境调控对提高CO2电还原效率的关键作用, 提供了一条具有工业应用潜力的CO2资源化利用新路径。