HZSM-5/SAPO-11复合分子筛的制备、表征及在异丁烷芳构化反应中的催化性能  

Preparation and Characterization of HZSM-5/SAPO-11 Composite Molecular Sieves and Their Catalytic Properties in Isobutane Aromatization

作　　者：张瑞珍[1,2] 温少波[1,2] 邢普[1,2] 赵欣[1,2] 王志翔[1,2] 韩培德[1,2] 赵亮富[3] ZHANG Ruizhen WEN Shaobo XING Pu ZHAO Xin WANG Zhixiang HAN Peide ZHAO Liangfu(College of Materials Science and Engineering Key Laboratory of InteqCuce Science and Engineering in Advanced Materials, Ministry of Education, Taiyuan University of Technology, Taiyuan 030024, China Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan 030001, China)

机构地区：[1]太原理工大学材料科学与工程学院 [2]新材料界面科学与工程教育部重点实验室,太原030024 [3]中国科学院山西煤炭化学研究所,太原030001

出　　处：《高等学校化学学报》2017年第1期126-132,共7页Chemical Journal of Chinese Universities

基　　金：国家自然科学基金(批准号:51371123);山西省基础研究项目(批准号:2014011002-1)资助~~

摘　　要：将经聚二烯丙基二甲基氯化铵(PDDA)预处理的HZSM-5分子筛置于SAPO-11分子筛的合成母液中,在水热体系中原位制备了一系列HZSM-5/SAPO-11复合分子筛,并对分子筛的结构、形貌及酸性进行了表征,考察了其在异丁烷芳构化反应中的催化性能.结果表明,所得复合分子筛由HZSM-5表面包覆约20 nm的SAPO-11微晶组成,且通过调变SAPO-11的Si含量可以有效调变复合分子筛的酸性,提高芳构化强弱酸协同催化作用,有效抑制裂解副反应.结合异丁烷芳构化转化率及液体收率结果可知,当SAPO-11合成溶胶中硅铝摩尔比为0.6时,HZSM-5/SAPO-11复合分子筛的芳构化活性及稳定性最佳.HZSM-5/SAPO-11 composite molecular sieves with different silicon contents were synthesized hydrothermally via in situ overgrowth of SAPO-11 on ZSM-5 pretreated by polydiallyldimethylammonium chloride（PDDA） , and were characterized by means of XRD, SEM, TEM, FTIR and NH3-TPD. The catalytic activity, stability and BTEX （benzene, toluene, ethylbenzene and xylenes） selectivity of HZSM-5/SAPO-11 in isobutane aromatization were also investigated. All the results were compared with those of ZSM-5, SAPO-11, and the mechanical mixtures of ZSM-5 and SAPO-11 and showed that the ZSM-5/SAPO-11 composites were composed of ZSM-5 covered by about 20 nm SAPO-11 round crystals, that modulation of ZSM-5/SAPO-11 acidity by altering Si content could effectively enhance the synergetic aromatization effect between strong and weak acids and restrain the cracking of iso-butane and the generation of C9＋, thus the liquid yield and stability of aromatization were superior to HZSM-5 and mechanical mixtures when the Si content reaches 0. 6 significantly.

关 键 词：HZSM-5/SAPO-11复合分子筛 异丁烷 芳构化 

分 类 号：O643[理学—物理化学]