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A New Family of Two-Dimensional Zeolites Prepared from the Intermediate Layered Precursor IPC-3P Obtained during the Synthesis of TUN Zeolite

机译:由TUN沸石合成过程中获得的中间层前体IPC-3P制备的二维沸石新家族

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摘要

The crystallization of zeolite TUN with 1,4-bis(N-methylpyrrolidinium)butane as template proceeds through an intermediate, designated IPC-3P, following the Ostwald rule of successive transformations. This apparently layered transient product has been thoroughly investigated and found to consist of MWW monolayers stacked without alignment in register, that is, disordered compared with MCM-22P. The structure was confirmed based on X-ray diffraction and high-resolution (HR)TEM analysis. The layered zeolite precursor IPC-3P can be swollen and pillared affording a combined micro- and mesoporous material with enhanced Brunauer-Emmett-Teller (BET) surface area (685m(2)g(-1)) and greater accessibility of BrOnsted acid sites for bulky molecules. This mesoporous material was probed with 2,6-di-tert-butylpyridine (DTBP). IPC-3P and its modification create a new layered zeolite sub-family belonging to the MWW family. FTIR data indicate that (Al)MWW materials MCM-22 and IPC-3 with Si/Al ratios greater than 20 exhibit a lower relative ratio of BrOnsted to Lewis acid sites than MCM-22 (with Si/Al ratios of around 13), that is, less than 2 versus more than 3, respectively. This is maintained even upon pillaring and warrants further exploration of materials like IPC-3P with a higher Al content. The unique XRD features of IPC-3P indicating misaligned stacking of layers and distinct from MCM-22P, are also seen in other MWW materials such as EMM-10P, hexamethonium-templated (HM)-MCM-22, ITQ-30, and UZM-8 suggesting the need for more detailed study of their identity and properties.
机译:遵循连续转化的Ostwald规则,以1,4-双(N-甲基吡咯烷鎓)丁烷为模板的TUN沸石的结晶通过称为IPC-3P的中间体进行。已经对这种表面明显的瞬态产物进行了彻底的研究,发现其由MWW单层组成,这些单层堆叠时没有对齐对齐,即与MCM-22P相比无序。基于X射线衍射和高分辨率(HR)TEM分析确认了该结构。可以对层状沸石前体IPC-3P进行溶胀和柱化处理,以提供具有增强的Brunauer-Emmett-Teller(BET)表面积(685m(2)g(-1))和更高的布朗斯泰德酸性位点可及性的微孔和中孔组合材料用于大分子。用2,6-二叔丁基吡啶(DTBP)探测该中孔材料。 IPC-3P及其修改版创建了一个属于MWW系列的新的层状沸石子系列。 FTIR数据表明,Si / Al比大于20的(Al)MWW材料MCM-22和IPC-3的布朗斯台德酸与路易斯酸位置的相对比比MCM-22低(Si / Al比约为13),即分别小于2和大于3。即使在立柱时也能保持这种状态,并保证进一步探索具有更高Al含量的材料,例如IPC-3P。 IPC-3P的独特XRD功能表明层错位堆叠且不同于MCM-22P,在其他MWW材料(例如EMM-10P,六甲铵模板(HM)-MCM-22,ITQ-30和UZM)中也可以看到-8表示需要对其身份和属性进行更详细的研究。

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