<p>The direct epoxidation of propylene to propylene oxide with hydrogen peroxide, known as the HPPO process, is a highly efficient and eco-friendly route for propylene oxide production. In the present study, the three-dimensional (3D) MWW-type titanosilicate Ti-MWW in shaped form was reconstructed to a 2D organic-inorganic hybrid material through the hydrothermal treatment of piperidine (PI) solution, which serves as a highly active catalyst for the fixed-bed HPPO process. The PI hydrothermal treatment induced chemical modifications on the Ti active centers, fabricating an open hexacoordinated Ti species [Ti(OSi)<sub>2</sub>(OH)<sub>2</sub>(H<sub>2</sub>O)PI], which significantly enhanced the catalytic activity. The solvent effect was also altered after the PI hydrothermal treatment, especially for methanol. In the continuous fixed-bed HPPO reaction, this 2D organic-inorganic Ti-MWW catalyst (RS-Ti-MWW) exhibited exceptional stability, achieving a lifetime of 730 h in MeCN and 216 h in MeOH, with PO selectivity exceeding 99.6% and H<sub>2</sub>O<sub>2</sub> utilization above 95%. RS-Ti-MWW can be regenerated through calcination and the subsequent hydrothermal treatment of PI solution, and the regenerated sample remains stable for up to 730 h of continuous operation, demonstrating its strong potential for industrial application.</p>

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Two-dimensional Organic-Inorganic Ti-MWW as Regenerable Catalyst for Fixed-bed Propylene Epoxidation

  • Liangliang Gong,
  • Xianchen Gong,
  • Jinpeng Yin,
  • Xintong Li,
  • Peng Wu,
  • Hao Xu

摘要

The direct epoxidation of propylene to propylene oxide with hydrogen peroxide, known as the HPPO process, is a highly efficient and eco-friendly route for propylene oxide production. In the present study, the three-dimensional (3D) MWW-type titanosilicate Ti-MWW in shaped form was reconstructed to a 2D organic-inorganic hybrid material through the hydrothermal treatment of piperidine (PI) solution, which serves as a highly active catalyst for the fixed-bed HPPO process. The PI hydrothermal treatment induced chemical modifications on the Ti active centers, fabricating an open hexacoordinated Ti species [Ti(OSi)2(OH)2(H2O)PI], which significantly enhanced the catalytic activity. The solvent effect was also altered after the PI hydrothermal treatment, especially for methanol. In the continuous fixed-bed HPPO reaction, this 2D organic-inorganic Ti-MWW catalyst (RS-Ti-MWW) exhibited exceptional stability, achieving a lifetime of 730 h in MeCN and 216 h in MeOH, with PO selectivity exceeding 99.6% and H2O2 utilization above 95%. RS-Ti-MWW can be regenerated through calcination and the subsequent hydrothermal treatment of PI solution, and the regenerated sample remains stable for up to 730 h of continuous operation, demonstrating its strong potential for industrial application.