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用B-ZSM-5沸石母体合成Ti-ZSM-5沸石用于丙烯环氧化

SYNTHESIS OF Ti-ZSM-5 ZEOLITE FOR PROPYLENE EPOXIDATION BY USING B-ZSM-5 ZEOLITE AS THE PRECURSOR

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【作者】 刘民郭新闻王祥生梁长海李灿

【Author】 LIU Min , GUO Xin-wen, WANG Xiang-sheng, LIANG Chang-hai, LI CanState Key Laboratory of Fine Chemicals . Dalian University of Technology , Dalian 116012 , China ; State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Dalian 116023, China)

【机构】 大连理工大学精细化工国家重点实验室大连化物所催化基础国家重点实验室大连化物所催化基础国家重点实验室 辽宁 大连 116012辽宁 大连 116012辽宁 大连 116023辽宁 大连 116023

【摘要】 以B-ZSM-5沸石为母体,经过脱硼处理后,在高温下与TiCl4进行气-固相取代合成钛硅沸石Ti-ZSM-5,考察了母体n(SiO2)/n(B2O3)对钛进入骨架的影响。以XRD、FT-IR、UV-Vis、XRF、Raman、ICP-AES和NH3程序升温脱附(TPD)等手段表征了催化剂,并考察了其丙烯环氧化性能。结果表明,随着母体n(SiO2)/n(B2O3)的增加,所制得的Ti-ZSM-5的n(SiO2)/n(TiO2)增大,即总钛含量降低;随着母体n(SiO2)/n(B2O3)的增加,所制备的Ti-ZSM-5的丙烯环氧化活性降低,而环氧丙烷的选择性增大。当以n(SiO2)/n(B2O3)=100的样品为母体时,制得Ti-ZSM-5中含有较多的锐钛矿型TiO2。

【Abstract】 Ti-ZSM-5 samples were successfully synthesized by using B-ZSM-5 with different n(SiO2)/w ( B2O3 ) ratios as precursors. The gas-solid synthesis of Ti-ZSM-5 included two steps: deboronated in HC1 solution firstly, then titanated with TiCl4. The effect of n(SiO2)/ n(B2O3) on the incorporation of titanium into the framework were investigated. The synthesized titanium- containing samples were thoroughly characterized by X-ray diffraction (XRD), Fourier-transformed infrared ( FT-IR ), X-ray fluorescence ( XRF), UV Vis spectroscopy, Raman spectroscopy, inductively coupled plasma-atomic emission spectroscopy (ICP-AES) and NH3 temperature programmed desorption (TPD). Propylene epoxidation properties were also investigated. The results showed that, n(SiO2 )/n(TiO2 ) in the product samples increased with the increase in the n(SiO2 )/n(B2O3) of the precursors; The conversion of H2O2 increased with the decrease of the n(SiO2 )/n(B2O3) of the precursor or the n(SiO2)/ n(TiO2) of the product, at the same time, the selectivity to propylene oxide (PO) decreased. Anatase appeared in Ti-ZSM-5 sample synthesized by using B-ZSM-5 with n(SiO2 )/n(B2O3) of 100 as the precursor.

【基金】 国家重点基础研究发展规划项目(G2000048009)
  • 【文献出处】 石油学报(石油加工) ,Acta Petrolei Sinica (Petroleum Processing Section) , 编辑部邮箱 ,2004年04期
  • 【分类号】O643.3
  • 【被引频次】28
  • 【下载频次】277
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