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<p>The electrocatalytic CO<sub>2</sub> reduction reaction (e-CO<sub>2</sub>RR) on Cu-based catalysts has been extensively studied; however, achieving high selectivity for C<sub>2+</sub> products and long-term durability remains challenging. Here, we introduce a straightforward approach that enhances both C<sub>2</sub>H<sub>4</sub> selectivity and catalyst durability by incorporating a nitrogen-rich Schiff-base Network (SNW), leveraging a synergistic interaction between Cu and SNW. Notably, Cu cubes with SNW, predominantly exposing the Cu(200) facet, achieve a Faradaic Efficiency (FE) of 71.2% for C<sub>2</sub>H<sub>4</sub> at a current density of 265 mA cm<sup>−2</sup>, which not only exceeds tetrahedral and spherical Cu with or without SNW, but also ranks competitively among state‑of‑the‑art Cu-based catalysts reported to date. Theoretical calculations suggest that the presence of SNW on Cu facilitates the *CO-*CHO coupling and/or the C<sub>2</sub>H<sub>4</sub> desorption, thereby enhancing C<sub>2</sub>H<sub>4</sub> formation. Furthermore, the Cu(200)-SNW surface exhibits optimized Gibbs free energies for the reaction steps compared to bare Cu and other SNW-modified Cu surfaces, which rationalizes the experimental observations. In situ electron microscopy further suggests that SNW confers durability by stabilizing Cu facets and preventing corrosion and dissolution under reaction conditions.</p>

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Synergistic surface modification of Cu with schiff-base networks for high selectivity and durability in CO2-to-C2H4 electroreduction

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年3月14日

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  • Wangjing Xie,
  • Tingting Tian,
  • Shengnan Yue,
  • Hualong Gu,
  • Ningning Shi,
  • Dechao Chen,
  • C. S. Praveen,
  • Xing Huang

摘要

The electrocatalytic CO2 reduction reaction (e-CO2RR) on Cu-based catalysts has been extensively studied; however, achieving high selectivity for C2+ products and long-term durability remains challenging. Here, we introduce a straightforward approach that enhances both C2H4 selectivity and catalyst durability by incorporating a nitrogen-rich Schiff-base Network (SNW), leveraging a synergistic interaction between Cu and SNW. Notably, Cu cubes with SNW, predominantly exposing the Cu(200) facet, achieve a Faradaic Efficiency (FE) of 71.2% for C2H4 at a current density of 265 mA cm−2, which not only exceeds tetrahedral and spherical Cu with or without SNW, but also ranks competitively among state‑of‑the‑art Cu-based catalysts reported to date. Theoretical calculations suggest that the presence of SNW on Cu facilitates the *CO-*CHO coupling and/or the C2H4 desorption, thereby enhancing C2H4 formation. Furthermore, the Cu(200)-SNW surface exhibits optimized Gibbs free energies for the reaction steps compared to bare Cu and other SNW-modified Cu surfaces, which rationalizes the experimental observations. In situ electron microscopy further suggests that SNW confers durability by stabilizing Cu facets and preventing corrosion and dissolution under reaction conditions.