分子筛合成中六亚甲基亚胺与环己胺二元胺的模板作用  

Templating Function of Hexamethyleneimine and Cyclohexylamine Binary Amines in Zeolite Synthesis

作　　者：牛雄雷[1] 谢素娟[1] 李宏冰[2] 姜天英[2] 徐龙伢[1] 

机构地区：[1]中国科学院大连化学物理研究所催化基础国家重点实验室 [2]中国石油天然气股份有限公司抚顺石化分公司,辽宁抚顺113008

出　　处：《催化学报》2005年第10期851-854,共4页

基　　金：国家重点基础研究发展计划(973计划)资助项目(2003CB615802)

摘　　要：以固体硅胶为硅源考察了六亚甲基亚胺(HMI)和环己胺(CHA)二元胺模板剂对分子筛合成产物的影响.XRD测试结果表明,当晶化温度为160℃,晶化时间为84 h,SiO2/Al2O3摩尔比为30,Na2O∶H2O∶(HMI+CHA)∶SiO2摩尔比为0.11∶45∶0.35∶1时,即使HMI仅占二元胺模板剂的25%(摩尔分数),所得分子筛仍为MCM-22;其它条件相同时,以单纯CHA为模板剂得到的是ZSM-35分子筛.用13C MAS NMR研究了HMI和CHA的状态,结果表明在单一HMI合成体系中,HMI既起MCM-22结构导向作用,又经质子化后起稳定骨架的作用;而在HMI和CHA二元胺体系中,HMI主要起结构导向作用,CHA则填充在MCM-22层间十元环中稳定骨架.The zeolite synthesis was carried out using hexamethyleneimine （HMI） and cyclohexylamine （CHA） binary amines as templates. The product is always MCM-22 under the conditions of SiO2/Al2O3 molar ratio of 30, Na2O： H2O： （HMI ＋ CHA） ：SiO2 molar ratio of 0.11：45：0.35 ： 1, crystallization time of 84 h and crystallization temperature of 160 ℃, even at a low HMI/CHA molar ratio of 1/3. The presence of CHA significantly enhances the relative crystallinity of MCM-22 at HMI/CHA ratios less than 1. However, CHA is an effective template to direct the formation of ZSM-35 crystals when it was used alone. ^13C MAS NMR spectra of HMI show some significant difference between the as-made MCM-22 samples obtained from the single HMI template matrix and the HMI-CHA binary amine template matrix. It is concluded that in the single HMI template system, HMI acts as a structure-directing agent as well as has a stabilizing effect on the pore structure in its protonized form; while in the HMI-CHA binary amine template system, HMI only plays a structure-directing role, and CHA stabilizes the framework of the MCM-22.

关 键 词：分子筛 MCM-22 ZSM-35 六亚甲基亚胺 环己胺 模板剂 

分 类 号：O624.6[理学—有机化学]