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<p>Bioelectrocatalytic CO<sub>2</sub> reduction offers a sustainable route for CO<sub>2</sub> bioconversion, yet remains limited by interfacial-intramolecular electron transfer and oxygen sensitivity. Here, we mine a formate dehydrogenase from <i>Shewanella oneidensis</i> MR-1 (<i>So</i>FdhAB) featuring completely oxygen tolerant and direct-electron-transfer (DET) electrocatalytic performances. Cryo-electron microscopy (Cryo-EM) analysis reveals an intramolecular electron highway comprising five [4Fe-4S] clusters, a regional face-face contact facilitating interfacial ET, and a unique oxygen resistance mechanism different from inactivation-activation. By acquiring a beneficial variant <i>So</i>FdhAB-Y94S, a direct bioelectrocatalytic CO<sub>2</sub> reduction system is constructed, accumulating 2.88 ± 0.03 mmol formate in 64 hours with a steady rate of 45.3 ± 0.5 μmol h<sup>−1</sup> cm<sup>−2</sup> and a Faradaic efficiency of 93.1 ± 5.2%. The merits of oxygen tolerance and efficient (electro)catalytic property endow <i>So</i>FdhAB a robust enzyme adopted in potential application scenarios, and the inherent DET capability may inspire the interfacial engineering of other oxidoreductases.</p>

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An interfacial-intramolecular electron highway for accelerated electrocatalytic CO2 reduction by an O2-tolerant formate dehydrogenase

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年3月3日

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  • Weisong Liu,
  • Peng Zhang,
  • Xiufeng Wang,
  • Kuncheng Zhang,
  • Wenhua Yang,
  • Huijuan Cui,
  • Jun Liu,
  • Junsong Sun,
  • Chun You,
  • Haiyang Cui,
  • Zhiguang Zhu,
  • Lingling Zhang

摘要

Bioelectrocatalytic CO2 reduction offers a sustainable route for CO2 bioconversion, yet remains limited by interfacial-intramolecular electron transfer and oxygen sensitivity. Here, we mine a formate dehydrogenase from Shewanella oneidensis MR-1 (SoFdhAB) featuring completely oxygen tolerant and direct-electron-transfer (DET) electrocatalytic performances. Cryo-electron microscopy (Cryo-EM) analysis reveals an intramolecular electron highway comprising five [4Fe-4S] clusters, a regional face-face contact facilitating interfacial ET, and a unique oxygen resistance mechanism different from inactivation-activation. By acquiring a beneficial variant SoFdhAB-Y94S, a direct bioelectrocatalytic CO2 reduction system is constructed, accumulating 2.88 ± 0.03 mmol formate in 64 hours with a steady rate of 45.3 ± 0.5 μmol h−1 cm−2 and a Faradaic efficiency of 93.1 ± 5.2%. The merits of oxygen tolerance and efficient (electro)catalytic property endow SoFdhAB a robust enzyme adopted in potential application scenarios, and the inherent DET capability may inspire the interfacial engineering of other oxidoreductases.