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<p>Electrocatalytic CO<sub>2</sub> reduction often suffers from competition with the hydrogen evolution reaction (HER), which lowers efficiency and limits product selectivity. Recent studies suggest that electron spin, when controlled at an electrode surface, can influence reaction pathways, but direct evidence linking spin effects to suppressed HER has been limited. Here we show that helical chiral copper (Cu) electrodes reduce competing HER during CO<sub>2</sub> reduction, consistent with spin polarization induced via the chiral-induced spin selectivity effect. The helically structured Cu electrodes are fabricated by electrodeposition with a chiral templating reagent. Time-resolved Kerr ellipticity measurements, which track spin-polarized carriers generated by an ultrafast Seebeck current, confirm spin accumulation at the chiral Cu surface. This spin polarization disfavours H–H bond formation, thereby suppressing HER and enabling formate production alongside CO. These findings demonstrate that chirality-based spin control offers a strategy for steering selectivity in CO<sub>2</sub> reduction and other reactions where HER is an undesired competitor.</p>

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Chirality-induced spin selectivity as a mechanism to control product selectivity during electrochemical CO2 reduction

  • 期刊论文

  • 发表日期：

    2026年5月12日

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  • Jeiwan Tan,
  • Jacob L. Shelton,
  • Demelza Wright,
  • Md Azimul Haque,
  • Simran S. Saund,
  • Debjit Ghoshal,
  • Trung H. Le,
  • Yifan Dong,
  • Michelle A. Smeaton,
  • Katherine L. Jungjohann,
  • Elisa M. Miller,
  • Matthew C. Beard,
  • Nathan R. Neale,
  • Jao van de Lagemaat

摘要

Electrocatalytic CO2 reduction often suffers from competition with the hydrogen evolution reaction (HER), which lowers efficiency and limits product selectivity. Recent studies suggest that electron spin, when controlled at an electrode surface, can influence reaction pathways, but direct evidence linking spin effects to suppressed HER has been limited. Here we show that helical chiral copper (Cu) electrodes reduce competing HER during CO2 reduction, consistent with spin polarization induced via the chiral-induced spin selectivity effect. The helically structured Cu electrodes are fabricated by electrodeposition with a chiral templating reagent. Time-resolved Kerr ellipticity measurements, which track spin-polarized carriers generated by an ultrafast Seebeck current, confirm spin accumulation at the chiral Cu surface. This spin polarization disfavours H–H bond formation, thereby suppressing HER and enabling formate production alongside CO. These findings demonstrate that chirality-based spin control offers a strategy for steering selectivity in CO2 reduction and other reactions where HER is an undesired competitor.