Citation: ZUO Yi, SONG Wan-Cang, WANG Meng-Li, XU Yong-Hai, WANG Xiang-Sheng, GUO Xin-Wen. Epoxidation of Propylene over Small-Crystal TS-1 Extrudate in a Fixed-Bed Reactor[J]. Acta Physico-Chimica Sinica, ;2013, 29(01): 183-190. doi: 10.3866/PKU.WHXB201211021 shu

Epoxidation of Propylene over Small-Crystal TS-1 Extrudate in a Fixed-Bed Reactor

1.
State Key Laboratory of Fine Chemicals, Department of Catalysis Chemistry and Engineering, Faculty of Chemical, Environmental and Biological Science and Technology, Dalian University of Technology, Dalian 116024, Liaoning Province, P. R. China

Received Date: 3 September 2012
Available Online: 2 November 2012
Fund Project: 新世纪优秀人才(NCET-04-0268) (NCET-04-0268)

A small-crystal titanium silicalite-1 (TS-1) with a size of 600 nm×400 nm×250 nm was synthesized using a nano-sized TS-1 mother liquor as the seed in a tetrapropyl ammonium bromide (TPABr)-ethylamine hydrothermal system, and was extruded with silica sol. The obtained TS-1 extrudate was characterized by X-ray powder diffraction (XRD), Fourier-transform infrared (FTIR) spectroscopy, ultraviolet-visible (UV-Vis) diffuse reflectance spectroscopy, and nitrogen physisorption. The reaction conditions, including temperature, pressure, molar ratio of propylene/H₂O₂ (n(C₃H₆)/n(H₂O₂)), the weight hourly space velocity (WHSV) of propylene, methanol and H₂O₂, and the concentration of NH₃·H₂O, were systematically studied to identify ideal condition propylene epoxidation over small-crystal TS-1 extrudate. The reaction temperature had little effect on the propylene oxide (PO) yield under the conditions examined. The highest PO yield was obtained when the pressure was 2.0 MPa and the n(C₃H₆)/n(H₂O₂) was 4. The PO content in the product was maximized when the WHSVs of propylene, methanol and H₂O₂ was 0.93, 2.5 and 0.25 h^-1respectively. A low concentration of NH₃·H₂O was beneficial for a high PO yield. Under the optimized condition, we compared catalytic performances of TS-1 with different crystal sizes and performed a long-term test over the small-crystal TS-1. The tests indicated that H₂O₂ conversion and PO selectivity could both reach 95%, even after 1000 h on stream.
- Epoxidation of propylene,
- TS-1,
- H₂O₂,
- Reaction condition,
- Characterization,
- Fixed-bed reactor
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