Synthesis and Advanced NMR Characterization of Ordered 3D Reticular Materials with PolySilicate Nodes and Hydrophobic OrganoSilicone Linkers

This work describes the synthesis of ordered 3D siloxane-silsesquioxane reticular materials with silicate D4R cubes (Si8O208−), harvested from a sacrificial tetrabutylammonium cyclosilicate hydrate (TBA-CySH) precursor, interlinked with octyl and dicyclopentyl (Cp2) hydrocarbon functionalities in a...

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Veröffentlicht in:Molecules (Basel, Switzerland) Jg. 30; H. 2; S. 228
Hauptverfasser: Jamoul, Jelle, Radhakrishnan, Sambhu, Houlleberghs, Maarten, Chandran, C. Vinod, Vits, Aline, Weckx, Pasquinel, Smet, Sam, Arenas Esteban, Daniel, Bals, Sara, Martens, Johan A., Breynaert, Eric
Format: Journal Article
Sprache:Englisch
Veröffentlicht: Switzerland MDPI AG 01.01.2025
MDPI
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ISSN:1420-3049, 1420-3049
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Zusammenfassung:This work describes the synthesis of ordered 3D siloxane-silsesquioxane reticular materials with silicate D4R cubes (Si8O208−), harvested from a sacrificial tetrabutylammonium cyclosilicate hydrate (TBA-CySH) precursor, interlinked with octyl and dicyclopentyl (Cp2) hydrocarbon functionalities in a one-step synthesis with organodichlorosilanes. Advanced solid-state NMR spectroscopy allowed us to unravel the molecular order of the nodes and their interconnection by the silicone linkers. In the case of octyl-methyl silicone linkers, changing the silane-to-silicate ratio in the synthesis allowed for tuning the length of the linker between the nodes. With dicyclopentyl linkers, the addition of dimethyldichlorosilane was essential to enable the formation of a reticular network. The resulting materials contained mixed, dimeric silicone linkers, i.e., Si8-O-Si(Me2)-O-Si(Cp2)-O-Si8.
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These authors contributed equally to this work.
ISSN:1420-3049
1420-3049
DOI:10.3390/molecules30020228