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<p>Electrically-powered synthesis provides a sustainable approach for propylene oxidation to propylene oxide and propylene glycol in aqueous medium using water as the oxygen source, which can substitute conventional energy-intensive process that relies on hazardous oxidants. However, current electrosynthesis is suffering from expensive catalysts, low current density and Faradaic efficiency. Herein, guided by accidental finding of Ag<sup>+</sup> showing activity for propylene electrooxidation to propylene glycol and following mechanistic understanding, we report 1,2,3-triazole-chelated Ag catalyst with improved current density (15.8 mA/cm<sup>2</sup>) and Faradaic efficiency (62.5%), comparable with heterogeneous Pt and Pd catalysts using 30-fold less expensive metal. We experimentally and theoretically demonstrate that triazole coordination modulates the oxidative ability of the in-situ formed Ag-oxo species, suppressing overoxidation and oxygen evolution. Furthermore, by employing a high-pressure electrolyzer, we strengthen propylene mass transfer and attain an enhanced current density of 61.1 mA/cm<sup>2</sup> with Faradaic efficiency of 73.4%. By circulating electro-deposition/dissolution of Ag, the catalyst shows reusability in 10 cycles. This work demonstrates the potential of using cost-effective homogeneous catalyst for propylene electrooxidation.</p>

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Homogeneous silver catalyst for propylene electrooxidation to propylene glycol

  • 期刊论文

  • 出版模式：

    开放获取

  • 发表日期：

    2025年11月24日

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  • Bo-Jun Yuan,
  • Si-Min Xu,
  • Xiang Liu,
  • An-Zhen Li,
  • Xi Wang,
  • Qiujin Shi,
  • Ruo-Pu Li,
  • Chunyu Zhang,
  • Xikang Zhao,
  • Jinyu Zheng,
  • Bi-Jie Li,
  • Haohong Duan

摘要

Electrically-powered synthesis provides a sustainable approach for propylene oxidation to propylene oxide and propylene glycol in aqueous medium using water as the oxygen source, which can substitute conventional energy-intensive process that relies on hazardous oxidants. However, current electrosynthesis is suffering from expensive catalysts, low current density and Faradaic efficiency. Herein, guided by accidental finding of Ag+ showing activity for propylene electrooxidation to propylene glycol and following mechanistic understanding, we report 1,2,3-triazole-chelated Ag catalyst with improved current density (15.8 mA/cm2) and Faradaic efficiency (62.5%), comparable with heterogeneous Pt and Pd catalysts using 30-fold less expensive metal. We experimentally and theoretically demonstrate that triazole coordination modulates the oxidative ability of the in-situ formed Ag-oxo species, suppressing overoxidation and oxygen evolution. Furthermore, by employing a high-pressure electrolyzer, we strengthen propylene mass transfer and attain an enhanced current density of 61.1 mA/cm2 with Faradaic efficiency of 73.4%. By circulating electro-deposition/dissolution of Ag, the catalyst shows reusability in 10 cycles. This work demonstrates the potential of using cost-effective homogeneous catalyst for propylene electrooxidation.