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分别采用1,4-(双乙氧基硅烷)苯(1,4-BTEB)和1,2-三乙氧基硅基乙烷(1,2-BTESE)作为有机硅源,正硅酸乙酯(TEOS)为无机硅源,钛酸四丁酯(TBOT)为钛源,以Pluronic EO20PO70EO20(P123)为模板剂在酸性环境下水热合成制备了Ti掺杂的有机-无机有序介孔有机硅材料Ti-SBA-15-ben和Ti-SBA-15-et.同时,在合成过程中加入H2O2作为配合剂调节钛源水解速度,制备得到Ti-SBA-15-ben-H和Ti-SBA-15-et-H.采用FT-IR、DR UV-Vis、N2物理吸附、XRD、TG-DSC、TEM等方法对制备的样品进行了表征.结果表明:合成过程中加入H2O2制备的苯基桥连有机硅杂化材料具有较好的疏水性能,其骨架中活性4价位钛含量高,结构有序性最好.在以叔丁基过氧化氢(TBHP)为氧源的环己烯氧化反应中对制备的催化材料进行了对比评价,结果表明:Ti-SBA-15-ben-H表现出最高的催化活性,其催化的反应以环氧化产物为主,环己烯的转化率为26.9%,环氧选择性为32.8%,T i-SBA-15-et催化的反应以烯丙位氧化产物2-环己烯-1-酮为主,环己烯的转化率为8.5%,2-环己烯-1-酮选择性为41.2%.
Using 1,4-BTEB and 1,2-BTESE as the organic silicon source, tetraethylorthosilicate (TEOS) as inorganic silicon source and tetrabutyl titanate (TBOT) as titanium source, Ti-doped organic-inorganic ordered mesoporous organosilicates were synthesized by hydrothermal synthesis using Pluronic EO20PO70EO20 (P123) Ti-SBA-15-ben and Ti-SBA-15-et. In the meantime, Ti-SBA-15-ben-H and Ti-SBA were prepared by adding H2O2 as a complexing agent to adjust the hydrolysis rate of Ti source -15-et-H.The prepared samples were characterized by FT-IR, DR UV-Vis, N2 adsorption, XRD, TG-DSC and TEM.The results showed that the synthesis of phenyl Bridged organosilicon hybrid materials have good hydrophobic properties, the framework of active 4 price titanium content is high, the best structural order in the tert-butyl hydroperoxide (TBHP) as the oxygen source of cyclohexene oxidation The results showed that Ti-SBA-15-ben-H showed the highest catalytic activity, the catalytic reaction was mainly epoxidation product, the conversion of cyclohexene was 26.9%, epoxy selectivity of 32.8 %, The reaction catalyzed by T i-SBA-15-et was mainly allylic oxidation product 2-cyclohexen-1-one, the conversion of cyclohexene was 8.5%, the yield of 2-cyclohexen- Selectivity was 41.2%.