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Abstract:

The complex cis-[Ru(Lpy)NO]3+ (I) (Lpy = N-(2-methylpyridyl)1,4,8,11-tetraazacyclotetradecane) was prepared by the stoichiometric reaction between Ru(dmso)4Cl2 and Lpy and an excess of NaNO2 in ethanolic medium, followed by acidification of the solution. The diamagnetic species was isolated as its hexafluorophosphate salt, and fully characterized by IR (νNO = 1917 cm-1) and diverse NMR techniques in combination with theoretical computations based on the density functional theory (DFT). The compound displays strong electronic transitions below 300 nm and weak ones in the visible region of the spectrum, all of them solvent insensitive. The reaction of cis-[Ru(Lpy)NO]3+ with OH- generates the strongly colored nitro compound cis-[Ru(Lpy)NO2]+ (II) The {RuNO}6 compound can be interconverted into the one-electron reduced {RuNO}7 species cis-[Ru(Lpy)NO]2+ (III). The reduction process is completely reversible in the cyclic voltammetry timescale with E0 (versus Ag/AgCl, 3 M Cl-) = -0.02 V and 0.18 V in water and acetonitrile, respectively. Controlled potential reduction in both solvents yields to the quantitative formation of III, a process which involves significant changes in the electronic spectroscopy. The {RuNO}7 species proved to be inert against ligand loss, and electrogenerated solutions remained unchanged for several hours if protected from atmospheric oxygen. Electrochemical reoxidation or exposure to air lead to the complete recovery of the starting cis-[Ru(Lpy)NO]3+ material, without signs of secondary reactions. The robustness of the coordination sphere appears as a consequence of the multidentate nature of Lpy. © 2007 Elsevier Ltd. All rights reserved.

Registro:

Documento: Artículo
Título:A new ruthenium nitrosyl species based on a pendant-arm 1,4,8,11-tetraazacyclotetradecane (cyclam) derivative: An experimental and theoretical study
Autor:De Candia, A.G.; Marcolongo, J.P.; Slep, L.D.
Filiación:Departamento de Química Inorgánica, Analítica y Química Física, INQUIMAE, Facultad de Ciencias Exactas, Pabellon 2, Ciudad Universitaria, C1428EHA Buenos Aires, Argentina
Palabras clave:Electronic structure; Nitrosyl; Redox conversion; Ruthenium; Spectroscopy
Año:2007
Volumen:26
Número:16
Página de inicio:4719
Página de fin:4730
DOI: http://dx.doi.org/10.1016/j.poly.2007.04.038
Título revista:Polyhedron
Título revista abreviado:Polyhedron
ISSN:02775387
CODEN:PLYHD
Registro:https://bibliotecadigital.exactas.uba.ar/collection/paper/document/paper_02775387_v26_n16_p4719_DeCandia

Referencias:

  • Richter-Addo, G.B., Legzdins, P., (1992) Metal Nitrosyls, , Oxford University Press, New York
  • Olabe, J.A., Slep, L.D., (2004) Comprehensive Coordination Chemistry II, from Biology to Nanotechnology, 1, p. 603. , Mc Cleverty J.A., and Meyer T.J. (Eds), Elsevier, Oxford
  • Enemark, J.H., Feltham, R.D., (1974) Coord. Chem. Rev., 13, p. 339
  • Enemark, J.H., Feltham, R.D., (1981) Top. Stereochem., 12, p. 155
  • Armor, N.J., Hoffman, M.Z., (1975) Inorg. Chem., 14, p. 444
  • Nagao, H., Nishimura, H., Funato, H., Ichikawa, Y., Howell, F.S., Mukaida, M., Kakihana, H., (1989) Inorg. Chem., 28, p. 3955
  • Nishimura, H., Matsuzawa, H., Togano, T., Mukaida, M., Kakihana, H., Bottomley, F., (1990) J. Chem. Soc., Dalton Trans., p. 137
  • Bottomley, F., (1978) Acc. Chem. Res., 11, p. 158
  • Gomes, M.G., Davanzo, C.U., Silva, S.C., Lopez, L.G.F., Santos, P.S., Franco, D.W., (1998) J. Chem. Soc., Dalton Trans., p. 601
  • Borges, S.D.S., Davanzo, C.U., Castellano, E.E., Z-Schpector, J., Silva, S.C., Franco, D.W., (1998) Inorg. Chem., 37, p. 2670
  • Gorelsky, S.I., DaSilva, S.C., Lever, A.B.P., Franco, D.W., (2000) Inorg. Chim. Acta, 300-302, p. 698
  • Baumann, F., Kaim, W., Baraldo, L.M., Slep, L.D., Olabe, J.A., Fiedler, J., (1999) Inorg. Chim. Acta, 285, p. 129
  • Wanner, M., Scheiring, T., Kaim, W., Slep, L.D., Baraldo, L.M., Olabe, J.A., Zalis, S., Baerends, E.J., (2001) Inorg. Chem., 40, p. 5704
  • Hauser, C., Glaser, T., Bill, E., Weyhermuller, T., Wieghardt, K., (2000) J. Am. Chem. Soc., 122, p. 4352
  • Roncaroli, F., Baraldo, L.M., Slep, L.D., Olabe, J.A., (2002) Inorg. Chem., 41, p. 1930
  • Roncaroli, F., Ruggiero, M.E., Franco, D.W., Estiu, G.L., Olabe, J.A., (2002) Inorg. Chem., 41, p. 5760
  • Videla, M., Jacinto, J.S., Baggio, R., Garland, M.T., Singh, P., Kaim, W., Slep, L.D., Olabe, J.A., (2006) Inorg. Chem., 45, p. 8608
  • McGarvey, B.R., Ferro, A.A., Tfouni, E., Bezerra, C.W.B., Bagatin, I., Franco, D.W., (2000) Inorg. Chem., 39, p. 3577
  • Li, M., Bonnet, D., Bill, E., Neese, F., Weyhermuller, T., Blum, N., Sellman, D., Wieghardt, K., (2002) Inorg. Chem., 41, p. 3444
  • Serres, R.G., Grapperhaus, C.A., Bothe, E., Bill, E., Weyhermuller, T., Neese, F., Wieghardt, K., (2004) J. Am. Chem. Soc., 126, p. 5138
  • Videla, M., Roncaroli, F., Slep, L.D., Olabe, J.A., (2007) J. Am. Chem. Soc., 129, p. 278
  • Frantz, S., Sarkar, B., Sieger, M., Kaim, W., Roncaroli, F., Olabe, J.A., Zalis, S., (2004) Eur. J. Inorg. Chem., p. 2902
  • Evans, I.P., Spencer, A., Wilkinson, G., (1973) J. Chem. Soc., Dalton Trans., p. 204
  • Meunier, I., Mishra, A.K., Hanquet, B., Cocolios, P., Guilard, R., (1995) Can. J. Chem., Rev. Can. Chim., 73, p. 685
  • Bard, A.J., Faulkner, L.R., (1980) Electrochemical Methods, Fundamentals and Applications, , John Wiley & Sons, Inc., New York
  • Noviandri, I., Brown, K.N., Fleming, D.S., Gulyas, P.T., Lay, P.A., Masters, A.F., Phillips, L., (1999) J. Phys. Chem. B, 103, p. 6713
  • Malinovsky, E.R., (1991) Factor Analysis in Chemistry. 2nd edn., , Wiley-Interscience, New York
  • Parise, A.R., Pollak, S., Slep, L.D., Olabe, J.A., (1995) An. Asoc. Quim. Argent., 83, p. 211
  • Frisch, M.J., (2004) Gaussian 03, Rev. D01, , Gaussian, Inc., Wallingford CT
  • Li, J., Noodleman, L., Case, D.A., (1999) Inorganic Electronic Structure and Spectroscopy, I, p. 661. , Solomon E.I., and Lever A.B.P. (Eds), John Wiley & Sons, New York
  • Curtis, N.F., (2004) Comprehensive Coordination Chemistry II, from Biology to Nanotechnology, 1, p. 447. , Mc Cleverty J.A., and Meyer T.J. (Eds), Elsevier, Oxford
  • Bottomley, F., (1989) Reactions of Coordinated Ligands, 2. , Braterman P.S. (Ed), Plenum Publ. Corp., New york
  • Bottomley, F., Mukaida, M., (1982) J. Chem. Soc., Dalton Trans., p. 1933
  • Ford, P.C., Lorkovic, I.M., (2002) Chem. Rev., 102, p. 993
  • Ford, P.C., Laverman, L., Lorkovic, I., (2003) Adv. Inorg. Chem., 54, p. 203
  • Lim, M.D., Lorkovic, I., Ford, P.C., (2005) J. Inorg. Biochem., 99, p. 151
  • Chevalier, A.A., Gentil, L.A., Olabe, J.A., (1991) J. Chem. Soc., Dalton Trans., p. 1959
  • Bosnich, B., Poon, C.K., Tobe, M.L., (1965) Inorg. Chem., 4, p. 1102
  • Szabo, A., Ostlund, N.S., (1989) Modern Quantum Chemistry. Introduction Advanced Electronic Structure Theory. 1st edn., , Dover Publications, Inc., Mineola, NY
  • Westcott, B.L., Enemark, J.H., (1999) Inorganic Electronic Structure and Spectroscopy, II, p. 403. , Solomon E.I., and Lever A.B.P. (Eds), John Wiley & Sons, New York
  • Lang, D.R., Davis, J.A., Lopes, L.G.F., Ferro, A.A., Vasconcellos, L.C.G., Franco, D.W., Tfouni, E., Clarke, M.J., (2000) Inorg. Chem., 39, p. 2294
  • Armor, J.N., Ha, S., Taube, H., (1968) J. Am. Chem. Soc., 90, p. 5928
  • Poon, C.K., Che, C.M., (1981) J. Chem. Soc., Dalton Trans., p. 1336
  • Tfouni, E., Ferreira, K.Q., Doro, F.G., da Silva, R.S., da Rocha, Z.N., (2005) Coord. Chem. Rev., 249, p. 405
  • Creutz, C., Chou, M.H., (1987) Inorg. Chem., 26, p. 2995
  • Creutz, C., Newton, M.D., Sutin, N., (1994) J. Photochem. Photobiol. A-Chem., 82, p. 47
  • Zwickel, A.M., Creutz, C., (1971) Inorg. Chem., 10, p. 2395
  • Shin, Y.G.K., Brunschwig, B.S., Creutz, C., Newton, M.D., Sutin, N., (1996) J. Phys. Chem., 100, p. 1104
  • Shin, Y.K., Brunschwig, B.S., Creutz, C., Sutin, N., (1996) J. Phys. Chem., 100, p. 8157
  • Slep, L.D., Olabe, J.A., (2001) J. Am. Chem. Soc., 123, p. 7186
  • da Silva, R.S., Gambardella, M.T.P., Santos, R.H.A., Mann, B.E., Tfouni, E., (1996) Inorg. Chim. Acta, 245, p. 215
  • da Silva, R.S., Tfouni, E., (1992) Inorg. Chem., 31, p. 3313
  • Baraldo, L.M., Bessega, M.S., Rigotti, G.E., Olabe, J.A., (1994) Inorg. Chem., 33, p. 5890
  • Estrin, D.A., Baraldo, L.M., Slep, L.D., Barja, B.C., Olabe, J.A., Paglieri, L., Corongiu, G., (1996) Inorg. Chem., 35, p. 3897
  • Gonzalez-Lebrero, M.C., Turjanski, A.G., Olabe, J.A., Estrin, D.A., (2001) J. Mol. Model., 7, p. 201
  • Bottomley, F., Crawford, J.R., (1972) J. Chem. Soc., Dalton Trans., p. 2145
  • Ford, P., Rudd, D.F.P., Gaunder, R., Taube, H., (1968) J. Am. Chem. Soc., 90, p. 1187
  • Tfouni, E., Krieger, M., McGarvey, B.R., Franco, D.W., (2003) Coord. Chem. Rev., 236, p. 57
  • Gutmann, V., (1976) Electrochim. Acta, 21, p. 661
  • Brunschwig, B.S., Creutz, C., Sutin, N., (1998) Coord. Chem. Rev., 177, p. 61

Citas:

---------- APA ----------
De Candia, A.G., Marcolongo, J.P. & Slep, L.D. (2007) . A new ruthenium nitrosyl species based on a pendant-arm 1,4,8,11-tetraazacyclotetradecane (cyclam) derivative: An experimental and theoretical study. Polyhedron, 26(16), 4719-4730.
http://dx.doi.org/10.1016/j.poly.2007.04.038
---------- CHICAGO ----------
De Candia, A.G., Marcolongo, J.P., Slep, L.D. "A new ruthenium nitrosyl species based on a pendant-arm 1,4,8,11-tetraazacyclotetradecane (cyclam) derivative: An experimental and theoretical study" . Polyhedron 26, no. 16 (2007) : 4719-4730.
http://dx.doi.org/10.1016/j.poly.2007.04.038
---------- MLA ----------
De Candia, A.G., Marcolongo, J.P., Slep, L.D. "A new ruthenium nitrosyl species based on a pendant-arm 1,4,8,11-tetraazacyclotetradecane (cyclam) derivative: An experimental and theoretical study" . Polyhedron, vol. 26, no. 16, 2007, pp. 4719-4730.
http://dx.doi.org/10.1016/j.poly.2007.04.038
---------- VANCOUVER ----------
De Candia, A.G., Marcolongo, J.P., Slep, L.D. A new ruthenium nitrosyl species based on a pendant-arm 1,4,8,11-tetraazacyclotetradecane (cyclam) derivative: An experimental and theoretical study. Polyhedron. 2007;26(16):4719-4730.
http://dx.doi.org/10.1016/j.poly.2007.04.038