An ordered mesoporous organosilica hybrid material with a crystal-like wall structure

An ordered mesoporous organosilica hybrid material with a crystal-like wall structure
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DOI:
10.1038/416304a
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发表时间:
2002-03-21
期刊:
影响因子:
64.8
通讯作者:
Terasaki, O
Terasaki, O
中科院分区:
综合性期刊1区
文献类型:
--
作者:
Inagaki, S;Guan, S;Terasaki, O

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表面活性剂介导的合成策略广泛用于制造金属氧化物(7)、金属(8)、碳(9)和混合有机二氧化硅(10-14)形式的有序中孔固体(1-6)。这些材料具有无定形孔壁,这可能限制它们的实际用途。在中孔金属氧化物的情况下,通过热处理(15,16)和水热处理(17)使骨架结构结晶的努力已经导致仅一部分孔壁结晶。在这里,我们报告的表面活性剂介导的有序的苯-二氧化硅杂化材料的合成,这种材料具有一个六方阵列的介孔与晶格常数为52.5埃,和晶体状的孔壁,表现出结构的周期性与间距为7.6埃沿着通道方向。周期性的孔表面结构的结果从交替的亲水和疏水层,分别由二氧化硅和苯。我们认为,这种材料是由于苯-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而形成的。我们期望其他有机二氧化硅和有机金属氧化物可以以类似的方式产生,以产生一系列具有分子尺度孔表面周期性的分级有序的中孔固体。
Surfactant-mediated synthesis strategies are widely used to fabricate ordered mesoporous solids(1-6) in the form of metal oxides(7), metals(8), carbon(9) and hybrid organosilicas(10-14). 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(15,16) and hydrothermal treatments(17) 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 Angstrom, and crystal-like pore walls that exhibit structural periodicity with a spacing of 7.6 Angstrom 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.