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Ion-Pairs in Aluminosilicate-Alkali Synthesis Liquids Determine the Aluminum Content and Topology of Crystallizing Zeolites
Chemistry of Materials ( IF 7.2 ) Pub Date : 2022-06-10 , DOI: 10.1021/acs.chemmater.2c00773
Karel Asselman 1 , Nick Pellens 1 , Barbara Thijs 1 , Nikolaus Doppelhammer 1, 2 , Mohamed Haouas 3 , Francis Taulelle 1, 4 , Johan A Martens 1, 4 , Eric Breynaert 1, 4 , Christine E A Kirschhock 1
Affiliation  

Using hydrated silicate ionic liquids, phase selection and framework silicon-to-aluminum ratio during inorganic zeolite synthesis were studied as a function of batch composition. Consisting of homogeneous single phasic liquids, this synthesis concept allows careful control of crystallization parameters and evaluation of yield and sample homogeneity. Ternary phase diagrams were constructed for syntheses at 90 °C for 1 week. The results reveal a cation-dependent continuous relation between batch stoichiometry and framework aluminum content, valid across the phase boundaries of all different zeolites formed in the system. The framework aluminum content directly correlates to the type of alkali cation and gradually changes with batch alkalinity and dilution. This suggests that the observed zeolites form through a solution-mediated mechanism involving the concerted assembly of soluble cation-oligomer ion pairs. Phase selection is a consequence of the stability for a particular framework at the given aluminum content and alkali type.

中文翻译:


铝硅酸盐碱合成液中的离子对决定结晶沸石的铝含量和拓扑结构



使用水合硅酸盐离子液体,研究了无机沸石合成过程中相选择和骨架硅铝比与批料组成的函数关系。该合成概念由均质单相液体组成,可以仔细控制结晶参数并评估产率和样品均匀性。构建了在 90°C 下合成 1 周的三元相图。结果揭示了批次化学计量和骨架铝含量之间依赖于阳离子的连续关系,该关系在系统中形成的所有不同沸石的相界上都有效。骨架铝含量与碱金属阳离子的类型直接相关,并随着批次碱度和稀释而逐渐变化。这表明观察到的沸石是通过溶液介导的机制形成的,涉及可溶性阳离子-低聚物离子对的协同组装。相选择是特定骨架在给定铝含量和碱类型下稳定性的结果。
更新日期:2022-06-10
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