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Abstract:

This work reports the preparation of a new 6-coordinated nitrosyl compound and its use as a model to explore the redox and acid-base properties of the three redox states of bound nitrosyl (formally NO+, NO •, NO-/HNO) in {RuNO}6,7,8 species. We prepared the octahedral {RuNO}6 complex [Ru(Me3[9] aneN3)(bpy)(NO)]3+ (Me3[9]aneN3: 1,4,7-trimethyl-1,4,7-triazacyclononane; bpy = 2,2′-bipyridine), and the related [Ru(Me3[9]aneN3)(bpy)(NO2)]+ nitro derivative. The compounds were characterized by chemical analysis, X-ray diffraction, NMR, IR, and UV-vis spectroscopies, cyclic voltammetry (CV), UV-vis/IR spectroelectrochemistry, and theoretical calculations (DFT, (TD)DFT). The reaction kinetics between the {RuNO}6 complex and the nucleophile OH- is also presented. The incorporation of tridentate and bidentate ligands in the coordination sphere prevents labilization issues associated with the trans effect when attaining the reduced states of the nitrosyl group. This allows for a consistent interpretation of the changes in the main geometrical parameters: Ru-N and N-O distances, Ru-N-O angle, and the νNO frequency and electronic transitions. We explore the redox properties in acetonitrile and aqueous solutions, and provide a potential (E1/2) - pH (Pourbaix) diagram for the three diatomic nitrosyl-bound species, as well as for HNO and NO2-, including the report of the pK a of the [Ru(Me3[9]aneN3)(bpy)(HNO)] 2+ ion, 9.78 ± 0.15 at 25.0 C. © 2014 American Chemical Society.

Registro:

Documento: Artículo
Título:Nitrosyl-centered redox and acid-base interconversions in [Ru(Me 3[9]aneN3)(bpy)(NO)]3,2,1+. The p K a of HNO for its nitroxyl derivative in aqueous solution
Autor:Codesido, N.O.; Weyhermüller, T.; Olabe, J.A.; Slep, L.D.
Filiación:Departamento de Química Inorgánica, Analítica y Química Física, 5 Universidad de Buenos Aires, Ciudad Universitaria, Pabellón 2, 3er piso, C1428EHA Ciudad Autónoma de Buenos Aires, Argentina
Max Planck Institute for Chemical Energy Conversion, Stiftstraße 34-36, D-45470 Mülheim am der Ruhr, Germany
Año:2014
Volumen:53
Número:2
Página de inicio:981
Página de fin:997
DOI: http://dx.doi.org/10.1021/ic402448p
Título revista:Inorganic Chemistry
Título revista abreviado:Inorg. Chem.
ISSN:00201669
CODEN:INOCA
Registro:https://bibliotecadigital.exactas.uba.ar/collection/paper/document/paper_00201669_v53_n2_p981_Codesido

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Citas:

---------- APA ----------
Codesido, N.O., Weyhermüller, T., Olabe, J.A. & Slep, L.D. (2014) . Nitrosyl-centered redox and acid-base interconversions in [Ru(Me 3[9]aneN3)(bpy)(NO)]3,2,1+. The p K a of HNO for its nitroxyl derivative in aqueous solution. Inorganic Chemistry, 53(2), 981-997.
http://dx.doi.org/10.1021/ic402448p
---------- CHICAGO ----------
Codesido, N.O., Weyhermüller, T., Olabe, J.A., Slep, L.D. "Nitrosyl-centered redox and acid-base interconversions in [Ru(Me 3[9]aneN3)(bpy)(NO)]3,2,1+. The p K a of HNO for its nitroxyl derivative in aqueous solution" . Inorganic Chemistry 53, no. 2 (2014) : 981-997.
http://dx.doi.org/10.1021/ic402448p
---------- MLA ----------
Codesido, N.O., Weyhermüller, T., Olabe, J.A., Slep, L.D. "Nitrosyl-centered redox and acid-base interconversions in [Ru(Me 3[9]aneN3)(bpy)(NO)]3,2,1+. The p K a of HNO for its nitroxyl derivative in aqueous solution" . Inorganic Chemistry, vol. 53, no. 2, 2014, pp. 981-997.
http://dx.doi.org/10.1021/ic402448p
---------- VANCOUVER ----------
Codesido, N.O., Weyhermüller, T., Olabe, J.A., Slep, L.D. Nitrosyl-centered redox and acid-base interconversions in [Ru(Me 3[9]aneN3)(bpy)(NO)]3,2,1+. The p K a of HNO for its nitroxyl derivative in aqueous solution. Inorg. Chem. 2014;53(2):981-997.
http://dx.doi.org/10.1021/ic402448p