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<p>Formaldehyde (FA) electrolysis is attractive for paired production of value‑added chemicals. However, conventional electrolysis adopts alkaline electrolytes, which triggers FA self-disproportionation and severe feed loss. Here we introduce a sustainable and selective strategy for valorizing FA through electrochemically mediated disproportionation in acidic electrolytes. By leveraging a dual-electrode system consisting of a hydrophobic copper tetraminophthalocyanine layer (CuTAPc-layer) cathode and a Pt<sub>2</sub>Ru bimetallic anode, we efficiently convert FA into methanol and formic acid at high Faradaic efficiencies of 93.2% and 91.3%, respectively. Compared with alkaline FA oxidation, which can lose up to 76% FA and complicate downstream separation, the acidic system suppresses side reactions to ensure high product purity. Mechanism studies reveal that the hydrophobic microenvironment of CuTAPc-layer suppresses hydrogen evolution, while the stronger oxophilicity of Pt<sub>2</sub>Ru enhances FA activation and lowers the key deprotonation barrier for FA oxidation. The integrated device demonstrates application potential in polyoxymethylene upgrading, delivering 374.2 mA at 4 V with ~90% single-pass conversion, establishing a scalable and eco-friendly electrochemical pathway for chemical upcycling.</p>

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Electrochemically mediated disproportionation for selective formaldehyde upcycling in acid

  • 期刊论文

  • 出版模式：

    开放获取

  • 发表日期：

    2026年3月18日

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  • Yun Song,
  • Zhaohua Zhu,
  • Tridip Das,
  • Aarya D. Riasati,
  • Jianjun Su,
  • Weihua Guo,
  • Yong Liu,
  • Geng Li,
  • Yinger Xin,
  • Qiang Zhang,
  • Mingming He,
  • Ruixuan Wang,
  • Rui Xue,
  • Shenlong Zhao,
  • Chuan Xia,
  • Ben Zhong Tang,
  • Marc Robert,
  • Xin Wang,
  • William A. Goddard III,
  • Ruquan Ye

摘要

Formaldehyde (FA) electrolysis is attractive for paired production of value‑added chemicals. However, conventional electrolysis adopts alkaline electrolytes, which triggers FA self-disproportionation and severe feed loss. Here we introduce a sustainable and selective strategy for valorizing FA through electrochemically mediated disproportionation in acidic electrolytes. By leveraging a dual-electrode system consisting of a hydrophobic copper tetraminophthalocyanine layer (CuTAPc-layer) cathode and a Pt2Ru bimetallic anode, we efficiently convert FA into methanol and formic acid at high Faradaic efficiencies of 93.2% and 91.3%, respectively. Compared with alkaline FA oxidation, which can lose up to 76% FA and complicate downstream separation, the acidic system suppresses side reactions to ensure high product purity. Mechanism studies reveal that the hydrophobic microenvironment of CuTAPc-layer suppresses hydrogen evolution, while the stronger oxophilicity of Pt2Ru enhances FA activation and lowers the key deprotonation barrier for FA oxidation. The integrated device demonstrates application potential in polyoxymethylene upgrading, delivering 374.2 mA at 4 V with ~90% single-pass conversion, establishing a scalable and eco-friendly electrochemical pathway for chemical upcycling.