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Cage-like Cu5Cs4-phenylsilsesquioxanes: synthesis, supramolecular structures, and catalytic activityстатья
Статья опубликована в высокорейтинговом журнале
Статья опубликована в журнале из списка Web of Science и/или Scopus- Авторы: Bilyachenko Alexey N., Arteev Ivan S., Khrustalev Victor N., Shul’pina Lidia S., Korlyukov Alexander A., Ikonnikov Nikolay S., Shubina Elena S., Kozlov Yuriy N., Conceição Nuno Reis, Guedes da Silva M.Fátima C, Mahmudov Kamran T., Pombeiro Armando J.L.
- Журнал: Inorganic Chemistry
- Том: 62
- Номер: 33
- Год издания: 2023
- Издательство: American Chemical Society
- Местоположение издательства: United States
- Первая страница: 13573
- Последняя страница: 13586
- DOI: 10.1021/acs.inorgchem.3c01989
- Аннотация: A small family of nonanuclear Cu5Cs4-based phenylsilsesquioxanes 1−2 were prepared by a convenient self-assembly approach and characterized by X-ray diffraction studies. The compounds 1 and 2 show some unprecedented structural features such as the presence of a [Ph14Si14O28]14− silsesquioxane ligand and a CuII5CsI4 nuclearity in which the metal cations occupy unusual positions within the cluster. Copper ions are “wrapped” into a silsesquioxane matrix, while cesium ions are located in external positions. This resulted in cesium-involved aggregation of coordination polymer structures. Both compounds 1 and 2 realize specific metallocene (cesium−phenyl) linkage between neighboring cages. Compound 2 is evaluated as a catalyst in the Baeyer−Villiger (B-V) oxidation of cyclohexanone and tandem cyclohexane oxidation/B-V oxidation of cyclohexanone with m-chloroperoxybenzoic acid (mCPBA) as an oxidant, in an aqueous acetonitrile medium, and HNO3 as the promoter. A quantitative yield of ε-caprolactone was achieved under conventional heating at 50 °C for 4 h or MW irradiation for 30 min (for cyclohexanone as substrate); 17 and 19% yields of lactone upon MW irradiation at 80 °C for 30 min and heating at 50 °C for 4 h, respectively (for cyclohexane as a substrate), were achieved. Complex 2 was evaluated as a catalyst for the oxidation of alkanes to alkyl hydroperoxides and alcohols to ketones with peroxides at 60 °C in acetonitrile. The maximum yield of cyclohexane oxidation products was 30%. Complex 2 exhibits high activity in the oxidation of alcohols.
- Добавил в систему: Астахов Григорий Сергеевич
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