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<p>Electrochemical CO<sub>2</sub> reduction reaction (CO<sub>2</sub>RR) to multi-carbon (C<sub>2+</sub>) products offers a promising solution for CO<sub>2</sub> valorization under ambient conditions. However, CO<sub>2</sub> reacts with highly alkaline cathodic microenvironments to form (bi)carbonates, compromising both CO<sub>2</sub> conversion efficiency and device lifespan. Acidic media can mitigate this issue but suffer from competing hydrogen evolution and sluggish C–C coupling, limiting activity and C<sub>2+</sub> selectivity. Here we show that surface-adsorbed iodide ions dramatically enhance CO<sub>2</sub>RR on copper in strong acids. When introduced via the electrolyte, iodide ions strongly interact with copper and remain adsorbed under CO<sub>2</sub>RR operating conditions. This results in a doubling of ethylene selectivity, a concurrent decrease in CO formation and a substantial reduction in overpotentials. Mechanistic studies reveal an unusual asymmetrical OC–COOH coupling pathway facilitated by iodide ions. With additional Ag alloying and electrolyte optimization, we achieve a high C<sub>2+</sub> partial current density of 940 mA cm<sup>−2</sup> at −1.08 V versus reversible hydrogen electrode, along with excellent stability.</p>

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Enhanced CO2 electroreduction to multi-carbon products in strong acid induced by surface-adsorbed iodide ions

  • 期刊论文

  • 发表日期：

    2025年12月2日

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  • Xue Ding,
  • Binbin Pan,
  • Baojie Fan,
  • Qinghan Yu,
  • Jie Xu,
  • Yuchen Yan,
  • Yuqing Luo,
  • Lu Wang,
  • Yanguang Li

摘要

Electrochemical CO2 reduction reaction (CO2RR) to multi-carbon (C2+) products offers a promising solution for CO2 valorization under ambient conditions. However, CO2 reacts with highly alkaline cathodic microenvironments to form (bi)carbonates, compromising both CO2 conversion efficiency and device lifespan. Acidic media can mitigate this issue but suffer from competing hydrogen evolution and sluggish C–C coupling, limiting activity and C2+ selectivity. Here we show that surface-adsorbed iodide ions dramatically enhance CO2RR on copper in strong acids. When introduced via the electrolyte, iodide ions strongly interact with copper and remain adsorbed under CO2RR operating conditions. This results in a doubling of ethylene selectivity, a concurrent decrease in CO formation and a substantial reduction in overpotentials. Mechanistic studies reveal an unusual asymmetrical OC–COOH coupling pathway facilitated by iodide ions. With additional Ag alloying and electrolyte optimization, we achieve a high C2+ partial current density of 940 mA cm−2 at −1.08 V versus reversible hydrogen electrode, along with excellent stability.