沸石晶体SAPO-34特殊的螺旋式生长结构研究  

Research on Special Spiral Growth Structure of Zeolite Crystals SAPO-34

作　　者：喜冬阳 颜婷婷[2] 樊旭峰[2] 马振宁[2] 苏锡国[2] 刘健[2] 

机构地区：[1]沈阳建筑大学材料科学与工程学院,辽宁沈阳110168 [2]沈阳建筑大学理学院,辽宁沈阳110168

出　　处：《沈阳建筑大学学报（自然科学版）》2017年第1期176-183,共8页Journal of Shenyang Jianzhu University：Natural Science

基　　金：国家自然科学基金青年科学基金项目(11604224);辽宁省教育厅基金项目(LJZ2016030;LJZ2016031);沈阳建筑大学科研基金青年基金项目(2015030);沈阳建筑大学学科涵育项目(XKHY2-101;XKHY2-105)

摘　　要：目的研究硅磷酸铝沸石在不同模板剂条件下的形貌特征,并寻求控制晶体形貌的方法,分析其生长机制及原理,并获得其形貌控制的规律.方法配制去离子水与磷酸的混合溶液,加入铝源拟薄水铝石,搅拌至完全溶解,再加入吗啉并搅拌,加入硅源白炭黑至产生均匀凝胶,加入适量氢氟酸,将凝胶转入配有聚四氟乙烯内衬的反应釜中晶化,过滤出固体产物,并用去离子水反复洗涤,放入烘箱干燥,并检测其XRD谱线、核磁谱线、扫描电镜图像及原子力显微镜图像.结果当n(HF)∶n(Al_2O_3)=0.4时,能够得到完整的螺旋式生长结构晶体,样品形貌最佳.结论氢氟酸中的氟离子通过与SAPO-34中的铝原子结合,一定程度上阻止了磷原子和铝原子的配位,改变了SAPO-34常规的层状生长机理,产生了特殊的螺旋式生长结构.The morphology characteristics of silicon aluminum phosphate zeolites under different templates were studied to seek for ways to control the crystal morphology. The mechanism and principles behind its growth were analyzed. And the key rules governing morphology control were acquired. The special zeolite crystals SAPO-34 was prepared by first mixing the deionized water with phosphoric acid and together with the aluminum source （pseudoboehmite）. Then morpholine was successively added into the above mixture. After that the silicon source （ fumed silica） was added slowly to the mixture. To make spiral growth structure of SAPO-34, subsequently, a certain amount of hydrofluoric acid （HF） was added at the end of the preparation. The final solution was loaded into the stainless steel autoclave. The product was separated and washed with deionized water for several times and then dried. Then the properties were investigated via in-situ X-ray diffraction （ XRD）, nuclear magnetism resonance （ NMR）, scanning electron microscopy （ SEM ）, and atomic force microscopy（AMF）. The experimental results indicate that when n（HF） ： n（Al2O3） = 0.4, the SAPO-34 crystals have the best and most complete of spiral shapes. The special spiral growth structure of zeolite crystals SAPO-34 observed in this study is attributed to the combination of fluoride ions and aluminum atoms, then partly stopping the coordination of phosphorus and aluminum atoms. So regular layer structure is changed and special spiral growth structure of zeolite crystals SAPO-34 is formed.

关 键 词：沸石晶体SAPO-34 吗啉 氢氟酸 螺旋式生长结构 生长机理 

分 类 号：O611.4[理学—无机化学]