Inagaki Shinji, Guan Shiyou, Ohsuna Tetsu, Terasaki Osamu
Toyota Central R&D Laboratories, Inc., Nagakute, Aichi, 480-1192, Japan.
Nature. 2002 Mar 21;416(6878):304-7. doi: 10.1038/416304a.
Surfactant-mediated synthesis strategies are widely used to fabricate ordered mesoporous solids in the form of metal oxides, metals, carbon and hybrid organosilicas. These materials have amorphous pore walls, which could limit their practical utility. In the case of mesoporous metal oxides, efforts to crystallize the framework structure by thermal and hydrothermal treatments have resulted in crystallization of only a fraction of the pore walls. Here we report the surfactant-mediated synthesis of an ordered benzene-silica hybrid material; this material has an hexagonal array of mesopores with a lattice constant of 52.5 A, and crystal-like pore walls that exhibit structural periodicity with a spacing of 7.6 A along the channel direction. The periodic pore surface structure results from alternating hydrophilic and hydrophobic layers, composed of silica and benzene, respectively. We believe that this material is formed as a result of structure-directing interactions between the benzene-silica precursor molecules, and between the precursor molecules and the surfactants. We expect that other organosilicas and organo-metal oxides can be produced in a similar fashion, to yield a range of hierarchically ordered mesoporous solids with molecular-scale pore surface periodicity.
表面活性剂介导的合成策略被广泛用于制备金属氧化物、金属、碳和杂化有机硅形式的有序介孔固体。这些材料具有无定形的孔壁，这可能会限制它们的实际应用。对于介孔金属氧化物，通过热处理和水热处理使骨架结构结晶的努力仅导致部分孔壁结晶。在此，我们报道了一种有序苯 - 二氧化硅杂化材料的表面活性剂介导合成；该材料具有晶格常数为52.5 Å的六边形介孔阵列，以及沿通道方向间距为7.6 Å的呈现结构周期性的类晶孔壁。周期性的孔表面结构是由分别由二氧化硅和苯组成的交替亲水层和疏水层导致的。我们认为这种材料是苯 - 二氧化硅前体分子之间以及前体分子与表面活性剂之间的结构导向相互作用的结果。我们期望可以以类似的方式制备其他有机硅和有机金属氧化物，以产生一系列具有分子尺度孔表面周期性的分级有序介孔固体。
