Preparation of hierarchical nano-SAPO-11 zeolites as catalystsfor the synthesis of 2,6-dimethylnaphthalene
ZHANG Xiaohua;ZHANG Pu;JI Lin;JIANG Lejie;SONG Yanping;WEI Haiguo;ZENG Qingfeng;YE Runping;FENG Gang
SAPO-11分子筛作为微孔沸石,通常粒径大,如何在水热法基础上进一步合成纳米多级孔SAPO-11分子筛极具挑战。在水热合成SAPO-11分子筛基础上,通过对前驱体凝胶进行老化处理制备纳米多级孔SAPO-11分子筛。其中,在80℃用搅拌老化制备的SAPO-11分子筛有最小晶体尺寸,通过SEM可知通过搅拌老化制备的S11-80℃-stirring分子筛呈现一种均匀纳米棒状结构,这些纳米棒的直径约500~700nm,长度约2~4μm。2-甲基萘(2-MN)主要来源于煤焦油,可用于制备2,6-二甲基萘(2,6-DMN),用于合成高端聚酯,为此将上述纳米多级孔SAPO-11分子筛用于催化2-甲基萘烷基化反应,结果表明使用老化处理制备的纳米多级孔SAPO-11分子筛有77.8%的2-MN初始转化率,20.4%的初始选择性,2,6-DMN、2,7-DMN的什么比为1.13,反应第4小时2,6-DMN选择性最高,为39.9%,通过系列表征揭示了纳米多级孔SAPO-11分子筛择形催化催化机理。
As a microporous zeolite, SAPO - 11 zeolites usually have a large particle size, but how to further synthesize hierarchicalnano-SAPO-11 zeolites on the basis of hydrothermal method is a great challenge. Based on the hydrothermal method,SAPO-11 zeoliteswere prepared by aging treatment with the precursor gel. Among them,the SAPO-11 zeolites prepared by stirring aging treatment at 80 ℃has the smallest crystal size. It can be seen by SEM that the S11-80 ℃ -stirring zeolite show a uniform nanorod-like structure,these nanorods have a diameter of about 500-700 nm and a length of about 2-4 μm. 2-Methylnaphthalene (2-MN),which is mainly derivedfrom coal tar,can be used to prepare 2,6-dimethylnaphthalene (2,6-DMN),and then be used to synthesize high-end polyester. Therefore,the above-mentioned hierarchical nano-SAPO-11 zeolites were applied to catalyze the alkylation reaction of 2-methylnaphthalene.The results show that the SAPO-11 zeolites prepared by aging treatment have 77.8% initial conversion of 2-MN,20.4% initial selectivity,1.13 ratio of 2,6- DMN / 2,7-DMN,and the highest selectivity of 2,6-DMN of 39.9% at the 4th hour of reaction. The shape selection catalytic mechanism of SAPO-11 molecular sieve was revealed by series characterization.
hierarchical pore;SAPO-11;aging treatment;alkylation;2,6-dimethylnaphthalene
主办单位:煤炭科学研究总院有限公司 中国煤炭学会学术期刊工作委员会