SSZ-13分子筛的蒸汽辅助法合成及晶化过程研究  

Research on the crystallization process in the synthesis of SSZ-13 zeolite by steam-assisted crystallization method

作　　者：刘瑞 张翊[1] 边慧敏 李若楠 李晓峰[2] 李玉平[1] 郭清萍[1] LIU Rui;ZHANG Yi;BIAN Hui-min;LI Ruo-nan;LI Xiao-feng;LI Yu-ping;GUO Qing-ping(College of Materials Science and Engineering,Taiyuan University of Technology,Taiyuan 030024,China;.2.Research Institute of Special Chemicals,Taiyuan University of Technology,Taiyuan 030024,China)

机构地区：[1]太原理工大学材料科学与工程学院,山西太原030024 [2]太原理工大学精细化工研究所,山西太原030024

出　　处：《天然气化工—C1化学与化工》2020年第2期24-28,89,共6页Natural Gas Chemical Industry

基　　金：国家自然科学基金(51371123);山西省基础研究项目(201701D121024);山西省回国人员资助项目(2017-042)。

摘　　要：以N,N,N-三甲基金刚烷胺(TMAdaOH)为模板剂,采用蒸汽辅助晶化法合成SSZ-13分子筛,研究合成过程中凝胶制备和晶化条件对产物影响。采用XRD、SEM、FT-IR和NH3-TPD等手段对合成样品的晶体结构、相对结晶度、形貌和酸量等进行表征,并考察了其在固定床反应器中甲醇制烯烃(MTO)反应中的催化性能。结果表明,蒸汽辅助晶化法合成过程中凝胶干燥温度和干燥时间对晶化过程有显著的影响,适当提高凝胶干燥温度和延长干燥时间,能够缩短SSZ-13分子筛的晶化时间;与水热法合成的样品H-SSZ-13相比较,蒸汽辅助晶化法合成样品S-SSZ-13晶粒尺寸更小更均匀,总酸量较低,在甲醇制取烯烃(MTO)反应中表现出更长的催化寿命与较高的双烯(乙烯+丙烯)选择性。SSZ-13 zeolites were synthesized by steam-assisted crystallization method with N,N,N-trimethylamine(TMAdaOH) as a template. The effects of gel preparation and crystallization conditions on the synthesis of SSZ-13 zeolite were investigated. The obtained SSZ-13 samples were characterized by XRD, SEM, FT-IR and NH3-TPD, and their structural, morphology and acidic properties were also discussed. The catalytic performances of the samples in methanol to olefins(MTO) reaction were evaluated in a fixed bed reactor. The results showed that the drying temperature and drying time during the steam assisted crystallization process had a significant effect on the crystallization. Increasing the gel drying temperature and prolonging the drying time could shorten the crystallization time of the SSZ-13 zeolite. Compared with the sample H-SSZ-13 obtained by the hydrothermal method, the sample S-SSZ-13 synthesized by steam-assisted crystallization method has smaller and more uniform crystal size, lower total acid content,longer catalytic life and higher total selectivity of ethylene and propylene in MTO reaction.

关 键 词：SSZ-13分子筛 CHA拓扑结构 晶化过程 蒸汽辅助法 甲醇制烯烃(MTO) 

分 类 号：O743[理学—晶体学] TQ426[化学工程]