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<p>Propylene oxide (PO) is a key industrial chemical, often produced by epoxidizing propylene with H<sub>2</sub>O<sub>2</sub> over titanium silicalite-1. However, current H<sub>2</sub>O<sub>2</sub> production via the anthraquinone process relies on fossil-derived hydrogen, leading to substantial CO<sub>2</sub> emissions. Sustainable PO synthesis requires green H<sub>2</sub>O<sub>2</sub> production. Here, we present a fully unassisted, solar- and bias-free system that generates H<sub>2</sub>O<sub>2</sub>. This platform enables modular, eco-friendly on-site PO synthesis by coupling formaldehyde oxidation with two-electron O<sub>2</sub> reduction under alkaline conditions. Efficient propylene epoxidation under these conditions is achieved using titanium silicalite-1 modified by introducing dinuclear titanium sites with Ti–O–Ti bonds, as revealed by density functional theory and instrumental analyses. The unassisted H<sub>2</sub>O<sub>2</sub> production system is integrated with the modified titanium silicalite-1 to realize continuous PO production (1657 μmol<sub>PO</sub> cm<sup>−2</sup> over 24 h), without electric or solar energy input. This unassisted PO production method can thus be energy-independent, offering a sustainable alternative to conventional processes.</p>

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Self-driven propylene epoxidation on modified titanium silicalite-1 by in situ generated hydrogen peroxide

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年9月30日

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  • Kwang Hyun Kim,
  • Seon Woo Hwang,
  • Taehyeon Kim,
  • Haneul Kim,
  • Myohwa Ko,
  • Sang Seok Yoon,
  • Min Seok Kang,
  • Wonjoo Jin,
  • Myung-Jun Kwak,
  • Tae Hoon Oh,
  • Kwanyong Seo,
  • Sung June Cho,
  • Ji-Wook Jang,
  • Ja Hun Kwak

摘要

Propylene oxide (PO) is a key industrial chemical, often produced by epoxidizing propylene with H2O2 over titanium silicalite-1. However, current H2O2 production via the anthraquinone process relies on fossil-derived hydrogen, leading to substantial CO2 emissions. Sustainable PO synthesis requires green H2O2 production. Here, we present a fully unassisted, solar- and bias-free system that generates H2O2. This platform enables modular, eco-friendly on-site PO synthesis by coupling formaldehyde oxidation with two-electron O2 reduction under alkaline conditions. Efficient propylene epoxidation under these conditions is achieved using titanium silicalite-1 modified by introducing dinuclear titanium sites with Ti–O–Ti bonds, as revealed by density functional theory and instrumental analyses. The unassisted H2O2 production system is integrated with the modified titanium silicalite-1 to realize continuous PO production (1657 μmolPO cm−2 over 24 h), without electric or solar energy input. This unassisted PO production method can thus be energy-independent, offering a sustainable alternative to conventional processes.