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<p>Direct electrochemical C–N coupling from abundant carbon and nitrogen sources offers a sustainable route for glycine synthesis, yet achieving high efficiency is challenging. This study developed an IL@Bi catalyst by anchoring ionic liquid (IL) 1-ethyl-2,3-dimethylimidazolium nitrate (EmmimNO<sub>3</sub>) on Bi. For the co-reduction of oxalic acid and NO<sub>3</sub><sup>−</sup>, the IL@Bi catalyst achieved a Faradaic efficiency toward glycine (FE<sub>glycine</sub>) of 81.1% with a current density of 286.2 mA cm<sup>−2</sup>, outperforming pristine Bi and reported state-of-the-art catalysts. Large-scale glycine synthesis was demonstrated, with a glycine production rate of 3.6 mol h<sup>−1</sup> g<sub>cat</sub><sup>−1</sup>. Using plasma-activated N<sub>2</sub> as the nitrogen source, glycine selectivity reached 89.0%. Mechanism studies demonstrated that oxalic acid and NO<sub>3</sub><sup>−</sup> were first reduced to glyoxylate oxime (GAO), which could be reduced to glycine after accepting electrons. On the IL@Bi catalyst, electron transfer followed a relayed mechanism, where electrons were initially transferred from Bi to Emmim<sup>+</sup>, forming the Emmim<sup><b>·</b></sup> radical, which then donated electrons to GAO, resulting in a faster conversion pathway than direct electron transfer from Bi to GAO and contributing to the outstanding catalytic performance.</p><p></p>

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Imidazolium radical-mediated electron transfer enhances electrochemical C–N coupling for glycine synthesis

  • 期刊论文

  • 发表日期：

    2025年9月18日

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  • Hengan Wang,
  • Yingying Cheng,
  • Yiyong Wang,
  • Ran Duan,
  • Meng Zhou,
  • Shiqiang Liu,
  • Wenling Zhao,
  • Huisheng Qin,
  • Jiahao Yang,
  • Yaguang Peng,
  • Lihong Jing,
  • Yi Xu,
  • Qinggong Zhu,
  • Xiaofu Sun,
  • Qingli Qian,
  • Jianling Zhang,
  • Xinchen Kang,
  • Buxing Han

摘要

Direct electrochemical C–N coupling from abundant carbon and nitrogen sources offers a sustainable route for glycine synthesis, yet achieving high efficiency is challenging. This study developed an IL@Bi catalyst by anchoring ionic liquid (IL) 1-ethyl-2,3-dimethylimidazolium nitrate (EmmimNO3) on Bi. For the co-reduction of oxalic acid and NO3−, the IL@Bi catalyst achieved a Faradaic efficiency toward glycine (FEglycine) of 81.1% with a current density of 286.2 mA cm−2, outperforming pristine Bi and reported state-of-the-art catalysts. Large-scale glycine synthesis was demonstrated, with a glycine production rate of 3.6 mol h−1 gcat−1. Using plasma-activated N2 as the nitrogen source, glycine selectivity reached 89.0%. Mechanism studies demonstrated that oxalic acid and NO3− were first reduced to glyoxylate oxime (GAO), which could be reduced to glycine after accepting electrons. On the IL@Bi catalyst, electron transfer followed a relayed mechanism, where electrons were initially transferred from Bi to Emmim+, forming the Emmim· radical, which then donated electrons to GAO, resulting in a faster conversion pathway than direct electron transfer from Bi to GAO and contributing to the outstanding catalytic performance.