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Abstract:

Quantum mechanical calculations at the density functional theory (DFT) level have been performed on diruthenium tetracarboxylates of different levels of molecular complexity: from unsolvated monomers to oligomers. The agreement between the calculated and experimental molecular structures and vibrational modes of the simple [Ru 2 (μ-O 2 CCH 3 ) 4 ] 0/ +and [Ru 2 (μ-O 2 CCH 3 ) 4 (H 2 O) 2 ] 10/+ systems made us confident in our calculation methodology. Therefore, it has been applied to the analysis of two different kinds of properties of these compounds: the trends in the UV/vis spectroscopy and electrochemistry along the [Ru 2 (μ-O 2 CCH 3 ) 4 X 2 ] - (X = Cl - , Br - , I) series, and the crystalline polymorphism related to the polymeric strand conformation in extended Ru 2 (μ-O 2 CR) 4 Cl compounds. For the [Ru 2 (μ-O 2 CCH 3 ) 4 X 2 ] - series, we report new spectroscopic and electrochemical results and interpret the trends on the basis of time dependent DFT-polarized continuum model calculations, local charge and spin analysis, and X donor properties. As far as the polymeric conformation is concerned, it has been previously suggested that the Ru-Cl-Ru angle results from a compromise between packing, orbital overlap, and microsegregation. Our calculations on [RU 2 (μ-O 2 CCH 3 ) 4 Cl] 2 Cl - and [Ru 2 (μ-O 2 CCH 3 ) 4 Cl] 3 Cl - oligomers provide insights on the influence of the first two factors on the strand conformation and allows a suggestion on what is the equatorial aliphatic chain's influence on this issue. © 2008 American Chemical Society.

Registro:

Documento: Artículo
Título:Theoretical and experimental studies of diruthenium tetracarboxylates structure, spectroscopy, and electrochemistry
Autor:Castro, M.A.; Roitberg, A.E.; Cukiernik, F.D.
Filiación:INQUIMAE, Departamento de Química Inorgánica, Analítica Y Química Física, Ciudad Universitaria, C1428EHA Buenos Aires, Argentina
Quantum Theory Project, University of Florida, Gainesville, FL 32611, United States
Instituto de Ciencias, Universidad Nacional de General Sarmiento, J. M. Gutierrez 1150, B1613GSX, Los Polvorines, Prov. Buenos Aires, Argentina
Año:2008
Volumen:47
Número:11
Página de inicio:4682
Página de fin:4690
DOI: http://dx.doi.org/10.1021/ic702505z
Título revista:Inorganic Chemistry
Título revista abreviado:Inorg. Chem.
ISSN:00201669
CODEN:INOCA
Registro:https://bibliotecadigital.exactas.uba.ar/collection/paper/document/paper_00201669_v47_n11_p4682_Castro

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Citas:

---------- APA ----------
Castro, M.A., Roitberg, A.E. & Cukiernik, F.D. (2008) . Theoretical and experimental studies of diruthenium tetracarboxylates structure, spectroscopy, and electrochemistry. Inorganic Chemistry, 47(11), 4682-4690.
http://dx.doi.org/10.1021/ic702505z
---------- CHICAGO ----------
Castro, M.A., Roitberg, A.E., Cukiernik, F.D. "Theoretical and experimental studies of diruthenium tetracarboxylates structure, spectroscopy, and electrochemistry" . Inorganic Chemistry 47, no. 11 (2008) : 4682-4690.
http://dx.doi.org/10.1021/ic702505z
---------- MLA ----------
Castro, M.A., Roitberg, A.E., Cukiernik, F.D. "Theoretical and experimental studies of diruthenium tetracarboxylates structure, spectroscopy, and electrochemistry" . Inorganic Chemistry, vol. 47, no. 11, 2008, pp. 4682-4690.
http://dx.doi.org/10.1021/ic702505z
---------- VANCOUVER ----------
Castro, M.A., Roitberg, A.E., Cukiernik, F.D. Theoretical and experimental studies of diruthenium tetracarboxylates structure, spectroscopy, and electrochemistry. Inorg. Chem. 2008;47(11):4682-4690.
http://dx.doi.org/10.1021/ic702505z