Journal
CHEMISTRY-A EUROPEAN JOURNAL
Volume 21, Issue 24, Pages 8758-8770Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/chem.201500791
Keywords
amidation; cage compounds; density functional calculations; metallacycles; oxidation
Categories
Funding
- Russian Foundation for Basic Research [12-03-00084-a, 14-03-00713, 14-03-31772]
- Council of the President of the Russian Federation [MD-3589.2014.3]
- Science without Borders Program, Brazil-Russia
- CAPES [A017-2013]
- Universite Montpellier 2
- Centre National de la Recherche Scientifique (CNRS), through the Groupe de Recherche International (GDRI) Homogenous catalysis for sustainable development (CH2D)
- French Embassy in Moscow
- Programme Andre Mazon
- Foundation for Science and Technology (FCT), Portugal [PTDC/QUI-QUI/121526/2010]
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The transmetalation of bimetallic copper-sodium silsesquioxane cages, namely, [(PhSiO1.5)(10)(CuO)(2)(NaO0.5)(2)] (Cooling Tower; 1), [(PhSiO1.5)(12)(CuO)(4)(NaO0.5)(4)] (Globule; 2), and [(PhSiO1.5)(6)(CuO)(4)(NaO0.5)(4)(PhSiO1.5)(6)] (Sandwich; 3), resulted in the generation of three types of hexanuclear cylinder-like copper silsesqui- oxanes, [(PhSiO1.5)(12)(CuO)(6)(C4H9OH)(2)(C2H5OH)(6)] (4), [(PhSiO1.5)(12)(CuO)(6)(C4H8O2)(4)(PhCN)(2)(MeOH)(4)] (5), and [(PhSiO1.5)(12)(CuO)(6)(NaCl)(C4H8O2)(12)(H2O)(2)] (6). The products show a prominent solvating system-structure dependency, as determined by X-ray diffraction. Topological analysis of cages 1-6 was also performed. In addition, DFT theory was used to examine the structures of the Cooling Tower and Cylinder compounds, as well as the spin density distributions. Compounds 1, 2, and 5 were applied as catalysts for the direct oxidation of alcohols and amines into the corresponding amides. Compound 6 is an excellent catalyst in the oxidation reactions of benzene and alcohols.
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