Interlayer Expansion of the Hydrous Layer Silicate RUB-36 to a Functionalized, Microporous Framework Silicate: Crystal Structure Analysis and Physical and Chemical Characterization
Interlayer Expansion of the Hydrous Layer Silicate RUB-36 to a Functionalized, Microporous Framework Silicate: Crystal Structure Analysis and Physical and Chemical Characterization
复制标题
含水层状硅酸盐 RUB-36 向功能化微孔骨架硅酸盐的层间膨胀：晶体结构分析和物理化学表征
DOI：
10.1021/cm300525u
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发表时间：
2012-04-24
影响因子：
8.6
通讯作者：
De Vos, Dirk
中科院分区：
文献类型：
--
作者：
Gies, Hermann;Mueller, Ulrich;De Vos, Dirk
含水层状硅酸盐RUB-36（C6 H16 N）（4）[H4 Si 36 O 76]已用于与二氯二甲基硅烷的层间膨胀反应，以将相邻的镁碱沸石型层互连成三维骨架硅酸盐。连接基团（-O-Si（CH 3）（2）-O-）仍具有合成形式的两个甲基（硅酸盐骨架的材料名称为COE-3 [Si 20 O38（CH 3）（4）]），从而提供疏水性质。层间膨胀沸石IEZ是热稳定的，并且可以在550 ℃下煅烧以产生亲水材料COE-4 [Si 20 O38（OH）（4）]。Si-29固态MAS NMR实验分别证实了制备和煅烧形式的连接基团的插入以及甲基和羟基取代。COE-3的BET表面积为238 m2/g，COE-4的BET表面积为350 m2/g。COE-3和COE-4在空间群Pm中结晶，其中a = 12.2503（3）埃，B = 13.9752（2）埃，c = 7.3850（1）埃，和β = 107.33（1）度和a = 12.16985（4）埃，B = 13.95066（3）埃，c = 7.37058（2）埃，和β = 107.30（1）度。COE-3和COE-4的PXRD图案的Rietveld晶体结构精修揭示了作为材料的均匀结构性质的包括连接基团的扩展的二维10环孔系统。
The hydrous layer silicate RUB-36, (C6H16N)(4) [H4Si36O76], has been used for an interlayer expansion reaction with dichlorodimethylsilane to interconnect neighboring ferrierite-type layers to a three-dimensional framework silicate. The linker group (-O-Si(CH3)(2)-O-) still has the two methyl groups in the as-synthesized form (material name COE-3 [Si20O38(CH3)(4)] for the silicate framework) rendering hydrophobic properties. The interlayer expanded zeolite, IEZ, is thermally stable and can be calcined at 550 degrees C to yield a hydrophilic material COE-4 [Si20O38(OH)(4)]. Si-29 solid state MAS NMR experiments confirm the insertion of the linker group and the methyl and hydroxyl substitution in the as-made and calcined form, respectively. The BET surface area is 238 m(2)/g for COE-3 and 350 m(2)/g for COE-4. COE-3 and COE-4 crystallize in space group Pm with a = 12.2503(3) angstrom, b = 13.9752(2) angstrom, c = 7.3850(1) angstrom, and beta = 107.33(1)degrees and a = 12.16985(4) angstrom, b = 13.95066(3) angstrom, c = 7.37058(2) angstrom, and beta = 107.30(1)degrees, respectively. Rietveld crystal structure refinement of the PXRD pattern of COE-3 and COE-4 reveal the expanded, two-dimensional 10-ring pore system including the linker group as homogeneous structural property of the materials.