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<p>Direct electrochemical epoxidation of alkenes could reduce the carbon intensity of epoxidation processes. However, highly selective electrified epoxidation is hindered by the competing oxygen evolution reaction. Analysis of the best-performing electrocatalysts reported to date reveals that propylene binds weakly to their surfaces while oxygen evolution intermediates predominate. Here we attempted to find catalysts on which surface-adsorbed propylene resides in proximity to reactive oxygen species. Screening a series of dopants revealed a volcano-type relationship between epoxidation activity and propylene adsorption, with indium-doped platinum–palladium oxide (In-PtPdOx) achieving the highest performance. The propylene oxide Faradaic efficiency reached 66% at 70 mA cm<sup>−2</sup> and 58% at 100 mA cm<sup>−2</sup>, with a high productivity of 1,080 μmol cm<sup>−2</sup> h<sup>−1</sup>. Integration into a membrane electrode assembly enabled a 46 wt% propylene oxide stream. Mechanistic characterization indicated that indium incorporation elevates the valence of platinum, strengthening metal–<i>π</i> C–C interactions with propylene and balancing propylene co-adsorption with reactive oxygen intermediates, thereby suppressing the oxygen evolution reaction and enabling highly selective epoxidation.</p><p></p>

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Electrified direct epoxidation of light hydrocarbons using alkene-binding atomic sites

  • 期刊论文

  • 发表日期：

    2026年6月25日

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  • Yongxiang Liang,
  • Yiqing Chen,
  • Yu Yang,
  • Rong Xia,
  • Jianan Erick Huang,
  • Zedong Zhang,
  • Bosi Peng,
  • Zeyan Liu,
  • Huajie Ze,
  • Aamir Hassan Shah,
  • Yali Ji,
  • Fengwang Li,
  • Ke Xie,
  • Edward H. Sargent

摘要

Direct electrochemical epoxidation of alkenes could reduce the carbon intensity of epoxidation processes. However, highly selective electrified epoxidation is hindered by the competing oxygen evolution reaction. Analysis of the best-performing electrocatalysts reported to date reveals that propylene binds weakly to their surfaces while oxygen evolution intermediates predominate. Here we attempted to find catalysts on which surface-adsorbed propylene resides in proximity to reactive oxygen species. Screening a series of dopants revealed a volcano-type relationship between epoxidation activity and propylene adsorption, with indium-doped platinum–palladium oxide (In-PtPdOx) achieving the highest performance. The propylene oxide Faradaic efficiency reached 66% at 70 mA cm−2 and 58% at 100 mA cm−2, with a high productivity of 1,080 μmol cm−2 h−1. Integration into a membrane electrode assembly enabled a 46 wt% propylene oxide stream. Mechanistic characterization indicated that indium incorporation elevates the valence of platinum, strengthening metal–π C–C interactions with propylene and balancing propylene co-adsorption with reactive oxygen intermediates, thereby suppressing the oxygen evolution reaction and enabling highly selective epoxidation.