首页> 外文期刊>Microporous and mesoporous materials: The offical journal of the International Zeolite Association >Interlayer expansion using metal-linker units: Crystalline microporous silicate zeolites with metal centers on specific framework sites
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Interlayer expansion using metal-linker units: Crystalline microporous silicate zeolites with metal centers on specific framework sites

机译:使用金属连接单元进行层间膨胀:具有金属中心位于特定骨架部位的结晶微孔硅酸盐沸石

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Interlayer expansion using silylating agents to connect layer silicates to 3D framework structures has shown to be a versatile synthesis route to new crystalline, microporous frameworks. We demonstrate here that also Me cations can be introduced on the linker sites applying the same synthesis procedure. An acidic aqueous Fe-chloride solution was used in a hydrothermal reaction to convert the layered hydrous silicate precursor RUB-36 into an interlayer expanded zeolite, containing Fe at the linker sites, Fe-IEZ-RUB-36, Si19.14Fe0.86O38(OH)(4). Structure analysis from powder X-ray data using the Rietveld technique confirmed that the porous framework is stable upon calcination and contains Fe on T-sites at the linker position. SEM-EDX analysis is in agreement with the analysis of the electron density maps showing that almost every other linker T-position is occupied by Fe-ions. The material crystallizes in the monoclinic space group Pm with a = 12.200(9) angstrom, b = 13.981(8) angstrom, c = 7.369(2) angstrom, and beta = 106.9(1)degrees. Applying a similar synthesis procedure, the Sn-analog, Sn-IEZ-RUB-36, Si38.6Sn1.4O76(OH)(8), has been obtained and structurally characterized. Despite its limited crystallinity, Rietveld analysis of the PXRD data set confirmed the materials framework topology and chemical composition (a = 23.856(14) angstrom, b = 14.103(7) angstrom, c = 7.412(7) angstrom, in SG Pnm2(1)). We conclude, that the synthesis procedure is flexible and, meanwhile, has been extended to other metal cations such as Ti, Zn, Eu and Al leading to microporous materials with potentially active metal cations on well defined sites of the silicate framework. (C) 2015 Elsevier Inc. All rights reserved.
机译:使用甲硅烷基化剂将层状硅酸盐连接到3D框架结构的层间扩展已显示是通向新的结晶微孔框架的通用合成途径。我们在这里证明,也可以使用相同的合成步骤在连接位点上引入Me阳离子。在水热反应中使用酸性Fe-氯化物水溶液将层状含水硅酸盐前体RUB-36转化为层间膨胀沸石,该沸石在连接位处Fe-IEZ-RUB-36,Si19.14Fe0.86O38( OH)(4)。使用Rietveld技术从粉末X射线数据进行结构分析,证实了多孔骨架在煅烧后是稳定的,并且在连接位的T位上含有Fe。 SEM-EDX分析与电子密度图的分析一致,表明几乎所有其他的接头T位置都被Fe离子占据。该材料在a = 12.200(9)埃,b = 13.981(8)埃,c = 7.369(2)埃和beta = 106.9(1)度的单斜空间群Pm中结晶。采用类似的合成方法,获得了Sn-类似物Sn-IEZ-RUB-36,Si38.6Sn1.4O76(OH)(8)并对其结构进行了表征。尽管结晶度有限,但Rietveld对PXRD数据集的分析仍确认了SG Pnm2(1 = 23.856(14)埃,b = 14.103(7)埃,c = 7.412(7)埃的材料构架拓扑和化学成分。 ))。我们得出结论,合成过程是灵活的,同时,它已扩展到其他金属阳离子,例如Ti,Zn,Eu和Al,从而导致在硅酸盐骨架的明确定义的位置上具有潜在活性金属阳离子的微孔材料。 (C)2015 Elsevier Inc.保留所有权利。

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