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作 者:金长子[1] 李钢[1] 王祥生[1] 王云[1] 马书启[1]
机构地区:[1]大连理工大学催化化学与工程系,辽宁大连116012
出 处:《石油学报(石油加工)》2005年第6期51-56,共6页Acta Petrolei Sinica(Petroleum Processing Section)
基 金:高等学校全国优秀博士学位论文作者专项资金(200346);中国石油天然气集团公司石油科技中青年创新基金(04E709)资助项目
摘 要:以十二胺为模板剂,正硅酸乙酯为硅源,钛酸四丁酯为钛源,于室温下合成了含Ti中孔分子筛Ti-HMS.通过改变Ti的用量得到了一系列不同硅/钛摩尔比(n(SiO2)/n(TiO2))的样品,采用XRD、TEM、XRF、UV-Vis等手段对这些样品进行表征;利用二苯并噻吩(DBT)和4,6-二甲基二苯并噻吩(4,6-DMDBT)氧化反应、丙烯环氧化反应、1-丁烯环氧化反应、环己酮氨氧化反应评价了所得样品的催化性能.结果表明,Ti-HMS分子筛多为20~70 nm的球状颗粒,且具有2~3 nm的蠕虫状(Worm-like)孔道;随着合成原料中Ti量的增加,进入Ti-HMS的骨架Ti量增多,但非骨架Ti也增多;随着骨架Ti含量的增加,样品的催化性能提高;Ti-HMS在大分子反应中的催化活性较高,在小分子反应中的催化活性不及TS-1.Ti-containing mesoporous molecular sieve Ti-HMS was synthesized at ambient temperature with dodecylamine as template, tetraethylorthosiliealite as Si source and tetrabutylorthotitanate as Ti source. The samples with different n(SiO2 )/n(TiO2 ) can be obtained through adding different amount of Ti source, which were characterized by XRD, TEM, XRF and UV-Vis. The catalytic performance of Ti-HMS was evaluated in the oxidation of DBT and 4, 6-DMDBT, the propylene epoxidation, the 1-butylene epoxidation and the ammoxidation of cyclohexanone. The results showed that the particles of Ti-HMS were spherical with the size of 20-70 nm and possessed worm-like channel with the size of 2-3 nm. With the increase of Ti content in raw materials, more Ti atoms entered the framework, and the Ti content of extra-framework also increased. Ti-HMS showed better catalytic performance in the oxidation of large molecules, but worse performance in small molecular reactions than TS-1.
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