异相晶种诱导快速合成低硅菱沸石分子筛
Rapid Synthesis of Low-Silica Chabazite Zeolite with the Addition of Heterogenous Seeds
作者单位E-mail
李玉琴 江西师范大学化学化工学院, 先进材料研究院, 分子筛膜材料国家地方联合工程实验室, 南昌 330022  
胡娜 江西师范大学化学化工学院, 先进材料研究院, 分子筛膜材料国家地方联合工程实验室, 南昌 330022  
张飞 江西师范大学化学化工学院, 先进材料研究院, 分子筛膜材料国家地方联合工程实验室, 南昌 330022  
朱美华 江西师范大学化学化工学院, 先进材料研究院, 分子筛膜材料国家地方联合工程实验室, 南昌 330022  
吴婷 江西师范大学化学化工学院, 先进材料研究院, 分子筛膜材料国家地方联合工程实验室, 南昌 330022  
陈祥树 江西师范大学化学化工学院, 先进材料研究院, 分子筛膜材料国家地方联合工程实验室, 南昌 330022 cxs66cn@jxnu.edu.cn 
摘要: 在不含有机模板剂体系(OSDAs)中,利用异相晶种(T型分子筛)诱导快速合成出纯相的低硅菱沸石分子筛。采用XRD、SEM、TEM、27Al MAS NMR和紫外拉曼等手段表征分子筛的结构属性和形貌特点。详细研究了菱沸石分子筛的晶化过程以及晶种添加量、nAl2O3/nSiO2nH2O/nSiO2和碱度对菱沸石分子筛晶化的影响,并探讨T型分子筛晶种诱导合成菱沸石分子筛的晶化机理。原位合成体系中仅形成L型分子筛晶相,而一定量T型分子筛异相晶种的加入诱导溶胶快速制备出纯相的菱沸石分子筛。T型分子筛晶体在一定的水热条件下不断溶解而释放的六元环(6R)和四元环(4R)迅速形成菱沸石分子筛特征笼(CHA笼),抑制了L型分子筛特征单元和特征笼(不含四元环的CAN笼)的形成。
关键词: 菱沸石分子筛  水热合成  异相晶种  无有机模板剂
基金项目: 国家自然科学基金(No.21476099和No.21766010)、国家国际科技合作专项(No.2015DFA50190)及江西省科技计划(No.20171BCB24005)资助项目。
Abstract: Pure-phase low-silica chabazite zeolites were rapidly synthesized by the addition of heterogenous seeds (zeolite T) without organic structural directing agents (OSDAs). Structural properties and morphology characteristics of the products were characterized using XRD, SEM, TEM, 27Al MAS NMR and UV Raman spectroscopy. Crystallization process of chabazite and the various parameters such as seed content, nAl2O3/nSiO2, nH2O/nSiO2 and alkalinity on the crystallization of crystals were investigated in detail. The formation mechanism of chabazite zeolite induced by zeolite T seed was also discussed. Only zeolite L was formed in the in-situ synthesis system while pure chabazite zeolite was fast obtained by adding a certain amount of zeolite T into the gel. The six-membered (6R) and four-membered rings (4R) released from the dissolved zeolite T under certain hydrothermal conditions rapidly formed the characteristic unit of chabazite zeolite (CHA cage), which inhibited the formation of the characteristic unit and characteristic cage of zeolite L (the CAN cage without four-membered ring).
Keywords: chabazite zeolite  hydrothermal synthesis  heterogenous seeds  OSDA-free
投稿时间:2018-06-27 修订日期:2018-08-26
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李玉琴,胡娜,张飞,朱美华,吴婷,陈祥树.异相晶种诱导快速合成低硅菱沸石分子筛[J].无机化学学报,2018,34(12):2143-2152.
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