<p>The electrosynthesis of amino acids represents a fascinating and promising frontier in green chemistry, offering a sustainable alternative to conventional industrial processes such as the energy-intensive Strecker synthesis through the adoption of efficient, electricity-driven methods. Herein, Sn is identified as an effective catalyst for glycine electrosynthesis using concentrated nitric acid and oxalic acid as feedstocks, and we investigate the reaction mechanism at industrial-level current rate (1 A cm<sup>-2</sup>). In-situ characterization reveals that the Sn undergoes dynamic valence cycle and reconstructs into amorphous-Sn under acidic conditions. At high current, the change in local pH promotes the anionic states of oxalic acid and C-intermediates, which enhances the adsorption of key intermediates such as glyoxalic acid and acid oxime. This switches the mechanism from a chain reaction to an interfacial hydrogenation, thereby increasing the rate of glycine formation. By increasing the dominance of interfacial reaction versus the chain reaction, we achieve a glycine Faradaic efficiency of 93%, and industrial-level partial current density of 0.9 A cm<sup>−2</sup> in a flow cell.</p>

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Sn catalyst reconstruction and microenvironment modulation for efficient amino acid electrosynthesis via C–N coupling

  • Shuhe Han,
  • Huimin Liu,
  • Janis Timoshenko,
  • Joonbaek Jang,
  • Mengyao Su,
  • Chenghua Sun,
  • Chengying Guo,
  • Yanmei Huang,
  • Arno Bergmann,
  • Beatriz Roldan Cuenya,
  • Yifu Yu,
  • Bin Zhang,
  • Kai Leng,
  • Kian Ping Loh

摘要

The electrosynthesis of amino acids represents a fascinating and promising frontier in green chemistry, offering a sustainable alternative to conventional industrial processes such as the energy-intensive Strecker synthesis through the adoption of efficient, electricity-driven methods. Herein, Sn is identified as an effective catalyst for glycine electrosynthesis using concentrated nitric acid and oxalic acid as feedstocks, and we investigate the reaction mechanism at industrial-level current rate (1 A cm-2). In-situ characterization reveals that the Sn undergoes dynamic valence cycle and reconstructs into amorphous-Sn under acidic conditions. At high current, the change in local pH promotes the anionic states of oxalic acid and C-intermediates, which enhances the adsorption of key intermediates such as glyoxalic acid and acid oxime. This switches the mechanism from a chain reaction to an interfacial hydrogenation, thereby increasing the rate of glycine formation. By increasing the dominance of interfacial reaction versus the chain reaction, we achieve a glycine Faradaic efficiency of 93%, and industrial-level partial current density of 0.9 A cm−2 in a flow cell.