A family of hexacopper phenylsilsesquioxane/acetate complexes: synthesis, solvent‐controlled cage structures, and catalytic activity

Zueva, A.Y.; Bilyachenko, A.; Arteev, I.S.; Khrustalev, V.N.; Dorovatovskii, P.V.; Shul’pina, L.S.; Ikonnikov, N.S.; Gutsul, E.I.; Rahimov, K.G.; Shubina, E.S.; Conceição, N.R.; Mahmudov, K.T.; Guedes da Silva, M.F.; Pombeiro Armando, J.L.

Авторы: Zueva Anna Y., Bilyachenko Alexey, Arteev Ivan S., Khrustalev Victor N., Dorovatovskii Pavel V., Shul’pina Lidia S., Ikonnikov Nikolay S., Gutsul Evgenii I., Rahimov Karim G., Shubina Elena S., Conceição Nuno Reis, Mahmudov Kamran T., Guedes da Silva M.Fátima C, Pombeiro Armando J.L.
Журнал: Chemistry - A European Journal
Том: 30
Номер: 31
Год издания: 2024
Издательство: John Wiley & Sons Ltd.
Местоположение издательства: United Kingdom
Номер статьи: e202401164
DOI: 10.1002/chem.202401164
Аннотация: Convenient self-assembly synthesis of copper(II) complexes via double (phenylsilsesquioxane and acetate) ligation allows to isolate a family of impressive sandwich-like cage compounds. An intriguing feature of these complexes is the difference in the structure of a pair of silsesquioxane ligands despite identical (Cu6) nuclearity and number (four) of acetate fragments. Formation of particular combination of silsesquioxane ligands (cyclic/cyclic vs condensed/condensed vs cyclic/condensed) was found to be dependent on the synthesis/crystallization media. A combination of Si4-cyclic and Si6-condensed silsesquioxane ligands is a brand new feature of cage metallasilsesquioxanes. A representative Cu6-complex (4) (with cyclic silsesquioxanes) exhibited high catalytic activity in the oxidation of alkanes and alcohols with peroxides. Maximum yield of the products of cyclohexane oxidation attained 30%. The compound 4 was also tested as catalyst in the Baeyer-Villiger oxidation of cyclohexanone by m-chloroperoxybenzoic acid: maximum yields of 88% and 100% of ε-caprolactone were achieved upon conventional heating at 50 °C for 4 h and MW irradiation at 70 or 80 °C during 30 min, respectively. It was also possible to obtain the lactone (up to 16% yield) directly from the cyclohexane via a tandem oxidation/Baeyer-Villiger oxidation reaction using the same oxidant.
Добавил в систему: Астахов Григорий Сергеевич

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A family of hexacopper phenylsilsesquioxane/acetate complexes: synthesis, solvent‐controlled cage structures, and catalytic activityстатья

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