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首页> 外文期刊>Chemistry: A European journal >Modified metal dibenzoylmethanates and their clathrates part III - Novel 4-vinylpyridine-extended metal-dibenzoylmethanate host frameworks: Structure, polymorphism, and inclusion properties
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Modified metal dibenzoylmethanates and their clathrates part III - Novel 4-vinylpyridine-extended metal-dibenzoylmethanate host frameworks: Structure, polymorphism, and inclusion properties

机译：改性的金属二苯甲酰甲烷酸盐及其包合物第三部分-新型的4-乙烯基吡啶延伸的金属-二苯甲酰甲烷酸酯主体构架：结构，多态性和包合性质

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摘要

In this contribution we show that host materials based on metal dibenzoylmethanates (DBM) can be extended in a versatile way by decreasing the packing efficiency of the simpler metal DBM's reported earlier. Specifically, this can be accomplished by coordinating two 4-vinylpyridines (4-ViPy) to the metal (Ni or Co) DBM units to give [M(4-ViPy)(2)(DBM)(2)] host complexes. These display a remarkable polymorphism and an ability to form inclusion compounds with a large variety of organic species, Five non-clathrate phases representing three polymorphic types and twenty-eight inclusion compounds with nineteen guests representing five structural types were isolated and studied in varying degrees of detail. The inclusion compounds can be prepared by recrystallization or by interaction of the solid host with guest vapor. In the latter case, the process realization, kinetics and final product strongly depend on the host polymorph chosen as starting material. Kinetic studies executed with powder XRD suggest that transient formation of inclusion compounds may occur even during solvent vapor induced transformation of one guest-free polymorph to another. The beta polymorph of the Ni-host reveals the strongest thratogenic ability as well as a high selectivity towards certain homologues and isomers. Its properties give insight into the concept of "flexible zeolite mimics", or "apohosts", as this empty host form is energetically and structurally predisposed towards inclusion processes. In all eleven (three host and eight clathrate) structures studied by single crystal X-ray diffraction the [M(4-Vi-Py)(2)(DBM)(2)] complex molecule is trans-configured. In most, the host molecules show effective packing in one dimension by forming parallel chains. Guest species are located between the chains in cages or channels formed by combining voids in the host molecules belonging to adjacent chains. The corresponding Ni and Co versions of the compounds studied were similar. [References: 75]
机译：在这一贡献中，我们表明，可以通过降低先前报道的较简单的金属DBM的包装效率，以通用的方式扩展基于金属二苯甲酰甲烷酸盐（DBM）的基质材料。具体而言，这可以通过将两个4-乙烯基吡啶（4-ViPy）与金属（Ni或Co）DBM单元配位以提供[M（4-ViPy）（2）（DBM）（2）]主体配合物来实现。它们显示出显着的多态性并能够形成具有多种有机物的包合物，分离并研究了代表三种多态类型的五个非包合物相和代表五种结构类型的十九种客体的二十八种包合物。详情。包合物可以通过重结晶或固体主体与客体蒸气的相互作用来制备。在后一种情况下，过程的实现，动力学和最终产物在很大程度上取决于选择作为起始原料的主体多晶型物。用粉末XRD进行的动力学研究表明，即使在溶剂蒸汽诱导的一种无客体多晶型物转化为另一种无定形物时，也可能会瞬时形成包合物。 Ni-主体的β多晶型物显示出最强的促生能力以及对某些同系物和异构体的高选择性。它的特性可以洞悉“柔性沸石模拟物”或“脱辅基”的概念，因为这种空的主体形式在能量和结构上都倾向于包含过程。在通过单晶X射线衍射研究的所有十一个（三个主体和八个包合物）结构中，[M（4-Vi-Py）（2）（DBM）（2）]复杂分子是反式构型的。在大多数情况下，宿主分子通过形成平行链在一维上显示出有效的堆积。客体物种位于笼子或通道中的链之间，该笼子或通道是通过合并属于相邻链的宿主分子中的空隙而形成的。所研究化合物的相应Ni和Co版本相似。 [参考：75]

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