模板剂对ZSM-5分子筛甲醛环化制三聚甲醛性能的影响  

Effect of templates in ZSM-5 zeolite on the reaction performance of formaldehyde cyclotrimerization to trioxane

作　　者：叶宇玲 雷骞[1] 陈洪林[1] 张小明[1] YE Yuling;LEI Qian;CHEN Honglin;ZHANG Xiaoming(Chengdu Institute of Organic Chemistry,Chinese Academy of Sciences,Chengdu 610041,Sichuan,China;College of Chemical Engineering,Sichuan University of Science&Engineering,Zigong 643000,Sichuan,China;University of Chinese Academy of Sciences,Beijing 100049,China)

机构地区：[1]中国科学院成都有机化学研究所,四川成都610041 [2]四川轻化工大学化工学院,四川自贡643000 [3]中国科学院大学,北京100049

出　　处：《化工进展》2020年第12期5049-5056,共8页Chemical Industry and Engineering Progress

基　　金：国家重点研发计划(2018YFB0604902)。

摘　　要：以四丙基氢氧化铵、四丙基溴化铵、正丁胺和季戊四醇为模板剂水热合成ZSM-5分子筛,采用XRF、XRD、SEM、NH_3-TPD、Py-FTIR和^(27)Al MAS NMR等进行了表征,研究了模板剂对ZSM-5分子筛性质及甲醛制三聚甲醛催化性能的影响。结果表明,通过改变模板剂可改变ZSM-5分子筛的酸中心分布、表面酸性质和粒径;较大空间的孔道交叉位置的酸性中心、小催化剂粒径和高表面B酸/L酸比值有利于提高三聚甲醛选择性。以四丙基氢氧化铵为模板剂合成的ZSM-5分子筛的颗粒尺寸为240nm×240nm×150nm,分布于直形孔道和S形孔道的孔道交叉处的Br?nsted酸中心较多,甲醛转化率和三聚甲醛的选择性分别为30.15%和88.35%。ZSM-5 zeolites were synthesized with different templates by hydrothermal method and characterized by XRF,XRD,SEM,NH3-TPD,Py-FTIR,and 27Al MAS NMR.The effect of templates on the catalytic performance of ZSM-5 zeolites in the trioxane synthesis was investigated.The results indicated that types of templates affected the distribution of acidity,the surface acidity and the particle size of the catalyst of the ZSM-5 zeolites.Acid sites located on the intersection of straight channel and S-channel,small particle size and high surface B acid/L acid ratio were favorable to enhancement of trioxane selectivity.Synthesized with tetrapropylammonium hydroxide,the ZSM-5 zeolite,of which the average particle size was 240nm×240nm×150nm and high acid sites distributed in the intersection of straight channel and S-channel,exhibited the formaldehyde conversion of 30.15%and trioxane selectivity of 88.35%.

关 键 词：三聚甲醛 ZSM-5分子筛 模板剂 酸分布 催化 

分 类 号：O643.3[理学—物理化学]