Hexacoppergermsesquioxanes as complexes with N-ligands: Synthesis, structure and catalytic properties

Kulakova, A.N.; Korlyukov, A.A.; Zubavichus, Y.V.; Khrustalev, V.N.; XavierBantrei; Shul'pina, L.S.; Levitsky, M.M.; Ikonnikov, N.S.; Shubina, E.S.; FrédéricLamaty; Bilyachenko, A.N.; Shul'pin, G.B.

Авторы: Kulakova Alena N., Korlyukov Alexander A., Zubavichus Yan V., Khrustalev Victor N., XavierBantrei, Shul'pina Lidia S., Levitsky Mikhail M., Ikonnikov Nikolay S., Shubina Elena S., FrédéricLamaty, Bilyachenko Alexey N., Shul'pin Georgiy B.
Журнал: Journal of Organometallic Chemistry
Том: 884
Год издания: 2019
Издательство: Elsevier BV
Местоположение издательства: Netherlands
Первая страница: 17
Последняя страница: 28
DOI: 10.1016/j.jorganchem.2019.01.004
Аннотация: A simple and versatile strategy of synthesis of cage metallagermaniumsesquioxanes is demonstrated for isolation of Cu6-based phenylgermsesquioxanes 1–6. Structure of newly synthesized coppergermsesquioxanes was established by single-crystal X-ray diffraction analysis. General principle of these cages' topology implies the presence of two linear Cu3 fragments, coordinated by three pairs of ligands. These are: (i) cyclic germsesquioxanes [PhGeO1,5]5, products 1–6, (ii) 1,10-phenanthrolines, (1, 3–5) or 2,2’-bipyridines, (2, 6), (or and (iii) OX species (X = H, 1–2, CH3, 3, H and C2H5O, 4, HCO, 5, CH3CO, 6). Appearance of non-expected species (formiate for 5, acetate for 6), resulted from corresponding alcohols used as reaction media, points at easyness of oxidation processes in the conditions of such self-assembling reactions. Catalytic tests showed high activity of complexes 1 and 2 as precatalysts in homogeneous oxidations of alkanes (cyclohexane, methylcyclohexane, n-heptane, cis-1,2-dimethylcyclohexane with hydrogen peroxide in acetonitrile solution. Hydroxyl radicals take part in the reaction. The same complexes catalyze oxidation of alcohols (cyclohexanol, 2-heptanol, 1-phenylethanol) to corresponding ketones with tert-butyl hydroperoxide in almost 100% yield. With the addition of various alkyl ammonium salts, complex 2 could also furnish corresponding amides in high yield.
Добавил в систему: Шульпин Георгий Борисович

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Hexacoppergermsesquioxanes as complexes with N-ligands: Synthesis, structure and catalytic propertiesстатья

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