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机构地区:[1]广东工业大学轻工化工学院,广东广州510090 [2]华南理工大学化工系,广东广州510641 [3]华南理工大学材料学院,广东广州510641
出 处:《石油学报(石油加工)》2005年第4期31-36,共6页Acta Petrolei Sinica(Petroleum Processing Section)
基 金:国家自然科学基金(20026005)资助项目
摘 要:采用阳离子表面活性剂十六烷基三甲基溴化铵(C16TMABr)与中性模板剂长链伯胺(CnNH2n+3)的混合物作为模板剂,通过带正电的表面活性剂胶束(S+)和带负电的硅物种(I-)之间的静电作用(即静电“S+I-”组装途径)合成了具有长程有序结构的Ti-MCM-41。CnNH2n+3的介入会影响C16TMABr胶团或液晶相的结构,可优化Ti-MCM-41的有序结构。合成凝胶中Ti与Si的摩尔比(vTi/vSi)、脂肪胺分子中碳原子数n(脂肪胺链长度)对中孔Ti-MCM-41骨架有序结构的形成有显著影响,只有在vTi/vSi<0.03、n<18范围内,才能够合成长程有序结构的Ti-MCM-41。在骨架Ti含量相近的情况下,采用混合模板法合成的Ti-MCM-41对于苯乙烯和环十二烯的催化氧化性能均优于单一表面活性剂模板法(分别采用静电“S+I-”和“S+X-I+”组装途径合成)合成的Ti-MCM-41。Ti-MCM-41 with long-ranged ordered structure was synthesized through the eleetrostatic interaction between positively charged surfactant micelles S^+ and anionic silicatespecies I^- (namely electrostatic “S^+ I^- ” assembly pathway)by using the mixture of cationic surfaetant C16 TMABr and neutral template CnNH2n+3 as template. Introduction of CnNH2n+3 into template influenced the structures of positively charged surfactant micelles S^+ or liquidcrystal phases, furtherly optimized the ordered structure of Ti-MCM-41. The VTi/VSi in gel, the number of carbon atoms(n) in the chain of CnNH2n+3 remarkably influenced the formation of long-ranged ordered structure of Ti-MCM-41. Only when VTi/vSi〈0. 03, n〈18, the long-range ordered Ti-MCM-41 could be obtained. Such long-range ordered Ti-MCM-41 synthesized by mixed templating method showed the higher catalytic activity to the oxidation reactions of styrene and cyclododecene than Ti-MCM-41 synthesized by single templating route under the condition of the similiar Ti contents in Ti-MCM-41 framework.
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