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<p>The electrochemical co-reduction of CO<sub>2</sub> and N<sub>2</sub> to urea presents a sustainable alternative to conventional synthesis but faces substantial challenges. Here we design a catalyst by anchoring the ionic liquid (IL) 1-ethyl-2,3-dimethylimidazolium bromide onto a CuBi surface. The IL@CuBi catalyst delivers an exceptional Faradaic efficiency toward urea (FE<sub>urea</sub>) of 73.0% and a current density of 27.4 mA cm<sup>−2</sup> in an H-type cell, with a production rate of 124.7 μmol cm<sup>−2</sup> h<sup>−1</sup>. Detailed study indicates that during the co-reduction process, Emmim<sup>+</sup> cations on IL@CuBi are first reduced to Emmim<sup>·</sup> radicals, which transfer electrons to H<sup>+</sup> to generate H<sup>·</sup> radicals. This relayed electron-transfer pathway for H<sup>·</sup> radical generation bypasses the conventional formation from surface-adsorbed *H intermediates, thereby effectively suppressing the hydrogen evolution reaction. The generated H<sup>·</sup> radicals, acting as high-energy bullets, directly participate in subsequent hydrogenation steps, thereby substantially reducing the free energy barrier and enhancing reaction kinetics.</p>

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A high-energy hydrogen radical initiates efficient electrosynthesis of urea from CO2 and N2

  • 期刊论文

  • 发表日期：

    2026年6月22日

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  • Hengan Wang,
  • Jiankang Liu,
  • Ran Duan,
  • Yiyong Wang,
  • Meng Zhou,
  • Shiqiang Liu,
  • Yaoyu Yin,
  • Huisheng Qin,
  • Ke Li,
  • Shipeng Zhang,
  • Xueqing Xing,
  • Qinggong Zhu,
  • Congyang Wang,
  • Xinchen Kang,
  • Buxing Han

摘要

The electrochemical co-reduction of CO2 and N2 to urea presents a sustainable alternative to conventional synthesis but faces substantial challenges. Here we design a catalyst by anchoring the ionic liquid (IL) 1-ethyl-2,3-dimethylimidazolium bromide onto a CuBi surface. The IL@CuBi catalyst delivers an exceptional Faradaic efficiency toward urea (FEurea) of 73.0% and a current density of 27.4 mA cm−2 in an H-type cell, with a production rate of 124.7 μmol cm−2 h−1. Detailed study indicates that during the co-reduction process, Emmim+ cations on IL@CuBi are first reduced to Emmim· radicals, which transfer electrons to H+ to generate H· radicals. This relayed electron-transfer pathway for H· radical generation bypasses the conventional formation from surface-adsorbed *H intermediates, thereby effectively suppressing the hydrogen evolution reaction. The generated H· radicals, acting as high-energy bullets, directly participate in subsequent hydrogenation steps, thereby substantially reducing the free energy barrier and enhancing reaction kinetics.