新型双核含芳环季铵盐模板剂的合成及分子筛的制备与应用

Preparation and Application of Zeolite Based on the Novel Binuclear Aromatic Quaternary Ammonium Template

本文报道了新型双核含芳环季铵盐化合物的合成,经核磁共振和红外光谱表征其结构,首次利用芳环季铵盐为模板剂,制备了具有MFI型衍射特征峰的新型ZSM-5分子筛,并借助XRD、SEM、N2吸附脱附、NH3-TPD等方法对其进行了表征。详细研究了该新型HZSM-5分子筛在缩酮反应中的催化性能,考察了分子筛用量、反应时间、温度等因素对缩酮反应的影响,优化了反应条件,并考察了该分子筛的循环使用效果。为进一步提高HZSM-5分子筛的催化活性,对其进行了质子交换改性,结果表明,改性后的HZSM-5分子筛具有催化活性高、稳定性好、重复使用次数多、催化剂分离方便、环境污染小等特点,是一种高效绿色的环保型固体酸。

A novel binuclear aromatic quaternary ammonium template was synthesized,and its structure was characterized by NMR and IR. On this basis,a new type of ZSM-5 zeolite with MFI-type diffraction peaks was prepared. The ZSM-5 zeolite was characterized by XRD,SEM,NH3 -TPD and N2 -adsorption-desorption. The novel HZSM-5 zeolite’s catalytic performance in condensation reaction of ethylene glycol and cyclohexanone was studied in detail. Then,the influences of zeolite dosage,reaction time and temperature on the Ketalization were investigated in order to optimize the reaction condition. Furthermore, the recycling of molecular sieve was organized under optimal reaction conditions. Subsequently,the HZSM-5 zeolite was modified by chlorosulfonic acid in order to improve the catalytic activity. After that,the ketalization catalyzed by the modified HZSM-5 zeolite under the optimal reaction conditions was investigated. The results revealed that the zeolite had high catalytic activity,good stability,easy recycling,easy separation of catalyst and few pollution,which can be used as an efficient and environmentally friendly green solid acid.