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<p>Electrochemical acetamide synthesis under ambient conditions offers a sustainable route for converting waste nitrate into valuable chemicals. Conventional methods, limited to standalone reduction or oxidation processes, typically achieve low Faradaic efficiencies (&lt;40%) and yields (&lt;0.2 mmol h⁻¹ cm⁻²). Here, we present a tandem reaction system coupling cathodic reduction and anodic oxidation in a full-cell electrolyzer to enhance acetamide production. At the cathode, nitrate is first reduced to nitrite, which subsequently oxidizes ethanol to acetaldehyde. This acetaldehyde reacts in situ with electrogenerated ammonia to form α-aminoethanol. The intermediate is then transported to the anode, where it undergoes oxidation to yield acetamide. The reaction pathway is confirmed through proton nuclear magnetic resonance spectroscopy, revealing efficient acetamide synthesis with a yield of 7.2 ± 0.3 mmol h⁻¹ (0.45 ± 0.02 mmol h⁻¹ cm⁻²) at a cell voltage of 2.4 V. Furthermore, the strategy extends to other amides, such as formamide and butyramide, underscoring its versatility. Techno-economic analysis highlights the viability of this route, with estimated production costs competitive against conventional thermal processes.</p>

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Coupling nitrate electrochemical reduction and nitrite oxidation of ethanol for acetamide synthesis

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年12月27日

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  • Qikun Hu,
  • Ouwen Peng,
  • Jia Liu,
  • Mengyao Su,
  • Junyuan Feng,
  • Kun Zhang,
  • Derong Chen,
  • Zong-Xiang Xu,
  • Kian Ping Loh

摘要

Electrochemical acetamide synthesis under ambient conditions offers a sustainable route for converting waste nitrate into valuable chemicals. Conventional methods, limited to standalone reduction or oxidation processes, typically achieve low Faradaic efficiencies (<40%) and yields (<0.2 mmol h⁻¹ cm⁻²). Here, we present a tandem reaction system coupling cathodic reduction and anodic oxidation in a full-cell electrolyzer to enhance acetamide production. At the cathode, nitrate is first reduced to nitrite, which subsequently oxidizes ethanol to acetaldehyde. This acetaldehyde reacts in situ with electrogenerated ammonia to form α-aminoethanol. The intermediate is then transported to the anode, where it undergoes oxidation to yield acetamide. The reaction pathway is confirmed through proton nuclear magnetic resonance spectroscopy, revealing efficient acetamide synthesis with a yield of 7.2 ± 0.3 mmol h⁻¹ (0.45 ± 0.02 mmol h⁻¹ cm⁻²) at a cell voltage of 2.4 V. Furthermore, the strategy extends to other amides, such as formamide and butyramide, underscoring its versatility. Techno-economic analysis highlights the viability of this route, with estimated production costs competitive against conventional thermal processes.