Preparation of Titanium Modified TUD-1 Catalysts for Propylene Epoxidation

Preparation of Titanium Modified TUD-1 Catalysts for Propylene Epoxidation
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钛改性TUD-1丙烯环氧化催化剂的制备

DOI:
10.1007/s10562-017-2030-8
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发表时间:
2017-03
期刊:
影响因子:
2.8
通讯作者:
Wu Jian
Wu Jian
中科院分区:
化学4区
文献类型:
--
作者:
Chen Jian;Fu Weiqin;Yuan Xia;Zeng Hongyan;Wu Jian

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摘要采用直接水热法合成了三维海绵状介孔Ti-TUD-1催化剂。通过控制钛源和硅源的水解,对其合成进行了改进,以将更多的四面体配位的Ti物种引入TUD-1基质的骨架中。通过XRD、FT-IR、ICP-AES、UV-Raman、UV-vis DRS、BJH/BET和29 Si MAS NMR等手段对催化剂进行表征,结果表明,在制备Ti-TUD-1催化剂的过程中,基质的加入顺序起着至关重要的作用,四面体配位的Ti物种的数量与基质的加入顺序密切相关。Ti物种的存在影响了TUD-1基质的内部结构和连通性。Ti-TUD-1催化剂具有较高的催化活性,特别是较好的PO选择性,这是由于四面体配位的Ti物种进入了TUD-1的骨架中。此外,还研究了TBOT/TEOS和TEA/TEOS摩尔比对催化活性的影响,表明适当的摩尔比促进催化活性的提高。Ti-TUD-1的织构性能与基体的加入顺序有关。通过控制钛源和硅源的水解,合成了Ti-TUD-1催化剂。四面体配位的Ti物种的数量也取决于衬底的添加顺序。图形摘要
AbstractA three-dimensional sponge-like mesoporous, Ti-TUD-1 catalyst was synthesized by a direct hydrothermal treatment method. Its synthesis was modified to introduce more tetrahedral-coordinated Ti species into the framework of TUD-1 matrix, by controlling the hydrolysis of titanium and silicon sources. The TUD-1 catalyst was characterized by XRD, FT-IR, ICP-AES, UV-Raman, UV–vis DRS, BJH/BET and29Si MAS NMR analyses, indicating that addition orders of substrate played a crucial role during the Ti-TUD-1 catalyst preparation, indicating the amount of tetrahedral-coordinated Ti species was closely related to the addition order of substrate. The presence of Ti species affected the internal structure and connectivity of TUD-1 matrix. The Ti-TUD-1 catalyst exhibited high catalytic activity, especially good PO selectivity, due to the tetrahedral-coordinated Ti species into the framework of TUD-1 matrix. Furthermore, the effect of the TBOT/TEOS and TEA/TEOS molar ratios, on the catalytic activity was also studied, demonstrating that adequate molar ratios promoted an improvement the catalytic activity. Textural properties of Ti-TUD-1 were related to the addition order of substrate. Ti-TUD-1 catalyst was synthesized by controlling the hydrolysis of titanium and silicon sources. Amount of tetrahedral-coordinated Ti species also depend on the addition order of substrate.Graphical Abstract
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