<p>Efficient CO<sub>2</sub> electroreduction to multi-carbon (C<sub>2+</sub>) oxygenates in acidic electrolytes remains a great challenge, especially under high current density conditions. In this study, we prepare an ionic liquid (IL)-modified Cu electrode (IL@Cu), which achieve a Faradaic efficiency (FE) of 82.7% toward C<sub>2+</sub> products at a current density of 2.0 A cm<sup>−2</sup> in 0.5 M K<sub>2</sub>SO<sub>4</sub> (pH = 1, adjusted with H<sub>2</sub>SO<sub>4</sub>), with a single-pass carbon efficiency reaching 78.5%. Under the same conditions, the partial current density for C<sub>2+</sub> oxygenates and ethanol exceed 1.2 A cm<sup>−2</sup> and 1.0 A cm<sup>−2</sup>, respectively, over IL@Cu. Mechanism study has shown that K<sup>+</sup> cations are repelled by the IL cations during the reaction, allowing water molecules to access the electrode surface. The displacement of K<sup>+</sup> enhances C–C coupling, while the proximity of water to the electrode surface facilitates the incorporation of oxygen-containing intermediates into the hydrogen bond network, thereby promoting the formation of C<sub>2+</sub> oxygenates.</p>

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Ampere-level CO2 electroreduction to multi-carbon oxygenates in acidic electrolyte through surface microenvironment reconstruction

  • Yaoyu Yin,
  • Zhongnan Ling,
  • Shiqiang Liu,
  • Shipeng Zhang,
  • Hengan Wang,
  • Wenling Zhao,
  • Huisheng Qin,
  • Rongjuan Feng,
  • Xueqing Xing,
  • Lihong Jing,
  • Yi Xu,
  • Qinggong Zhu,
  • Xiaofu Sun,
  • Qingli Qian,
  • Jianling Zhang,
  • Xinchen Kang,
  • Buxing Han

摘要

Efficient CO2 electroreduction to multi-carbon (C2+) oxygenates in acidic electrolytes remains a great challenge, especially under high current density conditions. In this study, we prepare an ionic liquid (IL)-modified Cu electrode (IL@Cu), which achieve a Faradaic efficiency (FE) of 82.7% toward C2+ products at a current density of 2.0 A cm−2 in 0.5 M K2SO4 (pH = 1, adjusted with H2SO4), with a single-pass carbon efficiency reaching 78.5%. Under the same conditions, the partial current density for C2+ oxygenates and ethanol exceed 1.2 A cm−2 and 1.0 A cm−2, respectively, over IL@Cu. Mechanism study has shown that K+ cations are repelled by the IL cations during the reaction, allowing water molecules to access the electrode surface. The displacement of K+ enhances C–C coupling, while the proximity of water to the electrode surface facilitates the incorporation of oxygen-containing intermediates into the hydrogen bond network, thereby promoting the formation of C2+ oxygenates.