具有聚硅酸盐节点和疏水性有机硅连接体的有序三维网状材料的合成与高级核磁共振表征
Synthesis and Advanced NMR Characterization of Ordered 3D Reticular Materials with PolySilicate Nodes and Hydrophobic OrganoSilicone Linkers.
作者信息
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
机构信息
Centre for Surface Chemistry and Catalysis-Characterization and Application Team (COK-KAT), KU Leuven, Celestijnenlaan 200F Box 2461, 3001 Heverlee, Belgium.
NMRCoRe-NMR/X-Ray Platform for Convergence Research, KU Leuven, Celestijnenlaan 200F Box 2461, 3001 Heverlee, Belgium.
出版信息
Molecules. 2025 Jan 8;30(2):228. doi: 10.3390/molecules30020228.
This work describes the synthesis of ordered 3D siloxane-silsesquioxane reticular materials with silicate D4R cubes (SiO), harvested from a sacrificial tetrabutylammonium cyclosilicate hydrate (TBA-CySH) precursor, interlinked with octyl and dicyclopentyl (Cp) 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., Si-O-Si(Me)-O-Si(Cp)-O-Si.
这项工作描述了从牺牲性的水合四丁基铵环硅酸盐（TBA-CySH）前体中获得的具有硅酸盐D4R立方体（SiO）的有序3D硅氧烷-倍半硅氧烷网状材料的合成，该材料通过与有机二氯硅烷的一步合成法与辛基和二环戊基（Cp）烃官能团互连。先进的固态核磁共振光谱使我们能够揭示节点的分子排列及其通过硅氧烷连接体的互连情况。在辛基-甲基硅氧烷连接体的情况下，改变合成中的硅烷与硅酸盐的比例可以调节节点之间连接体的长度。对于二环戊基连接体，添加二甲基二氯硅烷对于形成网状网络至关重要。所得材料包含混合的二聚体硅氧烷连接体，即Si-O-Si（Me）-O-Si（Cp）-O-Si。
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