Kim Tae-Wan, Kleitz Freddy, Paul Blain, Ryoo Ryong
National Creative Research Initiative Center for Functional Nanomaterials, Department of Chemistry (School of Molecular Science-BK21), Korea Advanced Institute of Science and Technology, Daejeon.
J Am Chem Soc. 2005 May 25;127(20):7601-10. doi: 10.1021/ja042601m.
Assembly of mesostructured silica using Pluronic P123 triblock copolymer (EO(20)-PO(70)-EO(20)) and n-butanol mixture is a facile synthesis route to the MCM-48-like ordered large mesoporous silicas with the cubic Iad mesostructure. The cubic phase domain is remarkably extended by controlling the amounts of butanol and silica source correspondingly. The extended phase domain allows synthesis of the mesoporous silicas with various structural characteristics. Characterization by powder X-ray diffraction, nitrogen physisorption, scanning electron microscopy, and transmission electron microscopy reveals that the cubic Iad materials possess high specific surface areas, high pore volumes, and readily tunable pore diameters in narrow distribution of sizes ranging from 4 to 12 nm. Moreover, generation of complementary pores between the two chiral channels in the gyroid Iad structure can be controlled systematically depending on synthesis conditions. Carbon replicas, using sucrose as the carbon precursor, are obtained with either the same Iad structure or I4(1)/a (or lower symmetry), depending on the controlled synthesis conditions for silica. Thus, the present discovery of the extended phase domain leads to facile synthesis of the cubic Iad silica with precise structure control, offering vast prospects for future applications of large-pore silica materials with three-dimensional pore interconnectivity.
使用普朗尼克P123三嵌段共聚物(EO(20)-PO(70)-EO(20))和正丁醇混合物组装介孔二氧化硅,是一种简便的合成路线,可制备具有立方Iad介孔结构的类MCM - 48有序大孔二氧化硅。通过相应地控制丁醇和硅源的量,立方相域得到显著扩展。扩展的相域使得能够合成具有各种结构特征的介孔二氧化硅。通过粉末X射线衍射、氮气物理吸附、扫描电子显微镜和透射电子显微镜表征发现,立方Iad材料具有高比表面积、高孔体积,并且孔径易于调节,在4至12 nm的窄尺寸分布范围内。此外,根据合成条件,可以系统地控制螺旋状Iad结构中两个手性通道之间互补孔的生成。以蔗糖为碳前驱体,根据二氧化硅的控制合成条件,可获得具有相同Iad结构或I4(1)/a(或更低对称性)的碳复制品。因此,目前对扩展相域的发现导致了具有精确结构控制的立方Iad二氧化硅的简便合成,为具有三维孔互连性的大孔二氧化硅材料的未来应用提供了广阔前景。