From monomers to geometry-constrained molecules: One step further toward cyanide bridged wires

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We report on the synthesis and properties of a family of linear cyanide bridged mixed-valence heptanuclear complexes with the formula: trans-[L 4RuII{(μ-NC)FeIII(NC)4(μ-CN) RuIIL′4(μ-NC)FeIII(CN) 5}2]6- (with L and L′ a para substituted pyridine). We also report on the properties of a related pentan...

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Autor principal: Alborés, P.
Otros Autores: Slep, L.D, Eberlin, L.S, Corilo, Y.E, Eberlin, M.N, Benítez, G., Vela, M.E, Salvarezza, R.C, Baraldo, L.M
Formato: Capítulo de libro
Lenguaje:Inglés
Publicado: 2009
Acceso en línea:Registro en Scopus
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Biblioteca Central Dr. Luis F. Leloir (FCEN) de Universidad de Buenos Aires
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030 |a INOCA 
100 1 |a Alborés, P. 
245 1 5 |a From monomers to geometry-constrained molecules: One step further toward cyanide bridged wires 
260 |c 2009 
270 1 0 |m Baraldo, L. M.; Departamento de Química Inorgánica, Analítica y Química Física, INQUIMAE-CONICET, Ciudad Universitaria, Pabellón 2, 3er piso, C1 428EHA Buenos Aires, Argentina; email: baraldo@qi.fcen.uba.ar 
506 |2 openaire  |e Política editorial 
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504 |a The orientation of the cyanide bridge is expected from the connectivity in the precursors. In previous work we did not find isomerization of the cyanide bridge and in one case we have prepared the two possible isomers (see ref 5, The properties of the two isomers are quite distinctive, especially their redox behavior. Isomerization of the bridge results in an increase in the redox potential of the RuII/III couple, while the FeIII/II couples become more irreversible because of the lability of the Fe-N(nitrile) bond. Our exploration of the redox properties of the complexes reported here show no evidence of bridge isomerization; Flanagan, J.B., Margel, S., Bard, A.J., Anson, F.C., (1978) J. Am. Chem. Soc, 100, pp. 4248-4253 
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504 |a We estimate the distance between the redox centers as multiples of the Fe-Ru distance of 5.05 Å observed in the trinuclear compounds; Fraysse, S., Coudret, C., Launay, J.P., (2003) J. Am. Chem. Soc, 125, pp. 5880-5888 
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520 3 |a We report on the synthesis and properties of a family of linear cyanide bridged mixed-valence heptanuclear complexes with the formula: trans-[L 4RuII{(μ-NC)FeIII(NC)4(μ-CN) RuIIL′4(μ-NC)FeIII(CN) 5}2]6- (with L and L′ a para substituted pyridine). We also report on the properties of a related pentanuclear complex. These oligomers were purified by size exclusion chromatography, characterized by electrospray ionization (ESI) mass spectrometry and elemental analysis, and their linear shape was confirmed by scanning tunneling microscopy (STM). These complexes present a rich electrochemistry associated with the seven redox active centers. The redox potential split of identical fragments indicates that there is considerable communication along the cyanide bridged backbone of the compounds, even for centers more than 3 nm apart. This small attenuation of the interaction at long distances make these cyanide bridged compounds good candidates for molecular wires. Interestingly, the extent of the communication depends on the relative energy of the fragments, as evaluated by their redox potentials, providing a guide for improvement of this interesting property. © 2009 American Chemical Society.  |l eng 
593 |a Departamento de Química Inorgánica, Analítica y Química Física, INQUIMAE-CONICET, Ciudad Universitaria, Pabellón 2, 3er piso, C1 428EHA Buenos Aires, Argentina 
593 |a Instituto de Investigaciones Fisicoquimicas Teóricas y Aplicadas, INIFTA-CONICET- UNLP, Casilla de Correo 16, Sucursal 4, 1900 La Plata, Argentina 
593 |a ThoMSon Mass Spectrometry Laboratory, Institute of Chemistry, University of Campinas - UNICAMP Campinas, São Paulo 13083-970, Brazil 
700 1 |a Slep, L.D. 
700 1 |a Eberlin, L.S. 
700 1 |a Corilo, Y.E. 
700 1 |a Eberlin, M.N. 
700 1 |a Benítez, G. 
700 1 |a Vela, M.E. 
700 1 |a Salvarezza, R.C. 
700 1 |a Baraldo, L.M. 
773 0 |d 2009  |g v. 48  |h pp. 11226-11235  |k n. 23  |p Inorg. Chem.  |x 00201669  |w (AR-BaUEN)CENRE-60  |t Inorganic Chemistry 
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