Choi Minkee, Cho Hae Sung, Srivastava Rajendra, Venkatesan Chithravel, Choi Dae-Heung, Ryoo Ryong
National Creative Research Initiative Center for Functional Nanomaterials, and Department of Chemistry, Korea Advanced Institute of Science and Technology, Daejeon 305-701, Korea.
Nat Mater. 2006 Sep;5(9):718-23. doi: 10.1038/nmat1705. Epub 2006 Aug 6.
Zeolites are a family of crystalline aluminosilicate materials widely used as shape-selective catalysts, ion exchange materials, and adsorbents for organic compounds. In the present work, zeolites were synthesized by adding a rationally designed amphiphilic organosilane surfactant to conventional alkaline zeolite synthesis mixtures. The zeolite products were characterized by a complementary combination of X-ray diffraction (XRD), nitrogen sorption, scanning electron microscopy (SEM) and transmission electron microscopy (TEM). The analyses show that the present method is suitable as a direct synthesis route to highly mesoporous zeolites. The mesopore diameters could be uniformly tailored, similar to ordered mesoporous silica with amorphous frameworks. The mesoporous zeolite exhibited a narrow, small-angle XRD peak, which is characteristic of the short-range correlation between mesopores, similar to disordered wormhole-like mesoporous materials. The XRD patterns and electron micrographs of the samples taken during crystallization clearly showed the evolution of the mesoporous structure concomitantly to the crystallization of zeolite frameworks. The synthesis of the crystalline aluminosilicate materials with tunable mesoporosity and strong acidity has potentially important technological implications for catalytic reactions of large molecules, whereas conventional mesoporous materials lack hydrothermal stability and acidity.
沸石是一类结晶铝硅酸盐材料,广泛用作择形催化剂、离子交换材料以及有机化合物吸附剂。在本研究中,通过向传统碱性沸石合成混合物中添加合理设计的两亲性有机硅烷表面活性剂来合成沸石。采用X射线衍射(XRD)、氮吸附、扫描电子显微镜(SEM)和透射电子显微镜(TEM)等多种手段对沸石产物进行表征。分析表明,该方法适合作为一种直接合成高介孔沸石的路线。介孔直径可以均匀调控,类似于具有无定形骨架的有序介孔二氧化硅。该介孔沸石呈现出一个窄的小角XRD峰,这是介孔之间短程相关性的特征,类似于无序的蠕虫状介孔材料。结晶过程中所取样品的XRD图谱和电子显微镜照片清楚地表明,介孔结构的演变与沸石骨架的结晶同时发生。合成具有可调介孔率和强酸性的结晶铝硅酸盐材料对于大分子催化反应具有潜在的重要技术意义,而传统介孔材料缺乏水热稳定性和酸性。