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Design of a Peripheral Building Block for H-Bonded Dendritic Frameworks and Analysis of the Void Space in the Bulk Dendrimers.

ABSTRACT: Three dendrimers, (t-Bu-G 2 N) 2 , CC(t-Bu-G 1 N) 3 and (t-Bu-G 1 N) 2 , with 3,5-di-tert-butyl amidobenzene as a common peripheral moiety were prepared in 64-83% yields and characterized. The bulk solids had high BET surface areas of 136-138?m2/g, which were similar for the three dendrimers in spite of their different molecular weight (ranging from 1791 to 2890). It was concluded that the peripheral amide groups do not imbed in the interstitial space of neighbouring dendrimer molecules but rather build a supramolecular architecture through strong intermolecular H-bonds. This mode of assembly generates voids in the bulk dendrimers responsible for sorption properties. The X-ray crystal structure analysis of a compound representing the peripheral moiety of the dendrimers and the FT-IR and powder-XRD data for (t-Bu-G 1 N) 2 suggest the proposed supramolecular structure. The isosteric heats of CO2 sorption (Q st) for (t-Bu-G 2 N) 2 were significantly higher than those for the other two dendrimers, which is consistent with the formation of a different type of voids within the interstitial space of the molecule. It is suggested that the interstitial void space can be designed and tuned to adjust its properties to a particular task, such as the separation of gases or a catalytic reaction facilitated by the dendrimer.

SUBMITTER: Lee CH

PROVIDER: S-EPMC5473840 | biostudies-other | 2017 Jun

REPOSITORIES: biostudies-other

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Design of a Peripheral Building Block for H-Bonded Dendritic Frameworks and Analysis of the Void Space in the Bulk Dendrimers.

Lee Cheng-Hua CH Soldatov Dmitriy V DV Tzeng Chung-Hao CH Lai Long-Li LL Lu Kuang-Lieh KL

Scientific reports 20170616 1

Three dendrimers, (t-Bu-G 2 N) 2 , CC(t-Bu-G 1 N) 3 and (t-Bu-G 1 N) 2 , with 3,5-di-tert-butyl amidobenzene as a common peripheral moiety were prepared in 64-83% yields and characterized. The bulk solids had high BET surface areas of 136-138 m2/g, which were similar for the three dendrimers in spite of their different molecular weight (ranging from 1791 to 2890). It was concluded that the peripheral amide groups do not ...[more]

PMID: 28623266

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Project description:We describe why the cyclic heteropolyanion [P8W48O184]40- (abbreviated as {P8W48}) is an ideal building block for the construction of intrinsically porous framework materials by classifying and analyzing >30 coordination polymers incorporating this polyoxometalate (POM) ligand. This analysis shows that the exocyclic coordination of first-row transition metals (TMs) to {P8W48} typically yields frameworks which extend through {W-O-TM-O-W} bridges in one, two, or three dimensions. However, despite the rich structural diversity of such compounds, the coordination of TMs to the {P8W48} ring is poorly understood, and therefore largely unpredictable, and had not until now been present with any structural classification that could allow rational design. Herein, not only do we present a new approach to understand and classify this new class of materials, we also present three {P8W48}-based frameworks which complement those frameworks which have previously been described. These new compounds help us postulate a new taxonomy of these materials. This is possible because the TM coordination sites of the {P8W48} ring are found, once fully mapped, to lead to well-defined classes of connectivity. Together, analysis provides insight into the nature of the building block connectivity within each framework, to facilitate comparisons between related structures, and to fundamentally unite this family of compounds. Hence we have tentatively named these compounds as "POMzites" to reflect the POM-based composition and zeolitic nature of each family member, although crucially, POMzites differ from zeolites in the modular manner of their preparation. As the synthesis of further POMzites is anticipated, the classification system and terminology introduced here will allow new compounds to be categorized and understood in the context of the established materials. A better understanding of TM coordination to the {P8W48} ring may allow the targeted synthesis of new frameworks rather than the reliance on serendipity apparent in current methods.

Dataset Information

Design of a Peripheral Building Block for H-Bonded Dendritic Frameworks and Analysis of the Void Space in the Bulk Dendrimers.

Publications

Design of a Peripheral Building Block for H-Bonded Dendritic Frameworks and Analysis of the Void Space in the Bulk Dendrimers.

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