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<p>Copper catalysts feature unique superiorities for the electrochemical conversion of CO<sub>2</sub> to C<sub>2+</sub> fuels and chemicals. Their surface oxidation states dominantly determine the reaction pathways to various products. However, most Cu-based catalysts inevitably undergo electroreduction from Cu<sup>2+</sup> to Cu<sup>1+</sup> or Cu<sup>0</sup> species during the electrochemical CO<sub>2</sub> reduction. Herein, we propose a straightforward strategy to stabilize Cu<sup>2+</sup> ions by coordinating them with benzobistriazole (H<sub>2</sub>BBTA), producing a metal-organic polymer (CuBBTA) with periodically adjacent copper atoms. Remarkably, CuBBTA delivers a high Faradaic efficiency of 62.0 ± 1.9% for CO<sub>2</sub>-to-C<sub>2</sub>H<sub>4</sub> conversion and a half-cell power conversion efficiency of 34.4% in a flow cell. It also maintains stable operation for over 50 hours in a zero-gap electrolyzer, sustaining a FE &gt; 55% at ≈ 1 A total current density. Operando X-ray absorption, Raman, and attenuated total reflection surface-enhanced infrared absorption spectroscopy (ATR-SEIRAS) reveal that the catalyst remains structurally stable with no dynamic transformation during the reaction. Online differential electrochemical mass spectrometry (DEMS), operando ATR-SEIRAS and theoretical calculations show that neighboring Cu<sup>2+</sup> ions in the polymer provide suitably-distanced dual sites that enable the energetically favorable formation of an <i>*</i>COCHO intermediate. This study presents a strategic method for developing stable catalysts for efficient CO<sub>2</sub>-to-ethylene electroconversion.</p>

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Operando insights on stable Cu2+ active sites for efficient electrochemical CO2-to-C2H4 conversion

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年3月13日

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  • Zonghang Zhang,
  • Qiang Xu,
  • Jingwei Han,
  • Ke Ren,
  • Yinmeng Hu,
  • Rui Zhao,
  • Hai Sun,
  • Jun-Sheng Qin,
  • Heng Rao

摘要

Copper catalysts feature unique superiorities for the electrochemical conversion of CO2 to C2+ fuels and chemicals. Their surface oxidation states dominantly determine the reaction pathways to various products. However, most Cu-based catalysts inevitably undergo electroreduction from Cu2+ to Cu1+ or Cu0 species during the electrochemical CO2 reduction. Herein, we propose a straightforward strategy to stabilize Cu2+ ions by coordinating them with benzobistriazole (H2BBTA), producing a metal-organic polymer (CuBBTA) with periodically adjacent copper atoms. Remarkably, CuBBTA delivers a high Faradaic efficiency of 62.0 ± 1.9% for CO2-to-C2H4 conversion and a half-cell power conversion efficiency of 34.4% in a flow cell. It also maintains stable operation for over 50 hours in a zero-gap electrolyzer, sustaining a FE > 55% at ≈ 1 A total current density. Operando X-ray absorption, Raman, and attenuated total reflection surface-enhanced infrared absorption spectroscopy (ATR-SEIRAS) reveal that the catalyst remains structurally stable with no dynamic transformation during the reaction. Online differential electrochemical mass spectrometry (DEMS), operando ATR-SEIRAS and theoretical calculations show that neighboring Cu2+ ions in the polymer provide suitably-distanced dual sites that enable the energetically favorable formation of an *COCHO intermediate. This study presents a strategic method for developing stable catalysts for efficient CO2-to-ethylene electroconversion.