Metallonitrosyl fragment as electron acceptor: intramolecular charge transfer, long range electronic coupling, and electrophilic reactivity in the trans-[NCRu(py)(4)(CN)Ru(py)(4)NO](3+) ion

Inorganic Chemistry
Federico RoncaroliJosé A Olabe

Abstract

The new complex trans-[NCRu(py)(4)(CN)Ru(py)(4)NO](PF(6))(3) (I) was synthesized. In acetonitrile solution, I shows an intense visible band (555 nm, epsilon = 5800 M(-1) cm(-1)) and other absorptions below 350 nm, associated with d(pi) --> pi(py) and pi(py) --> pi(py) transitions. The visible band is presently assigned as a donor-acceptor charge transfer (DACT) transition from the remote Ru(II) to the delocalized [Ru(II)-NO(+)] moiety. Photoinduced release of NO is observed upon irradiation at the DACT band. Application of the Hush model reveals strong electronic coupling, with H(DA) = approximately 2000 cm(-1). The difference between the optical absorption energy and redox potentials for the donor and acceptor sites (Ru(III,II), 1.40 V, and NO(+)/NO, 0.50 V, vs Ag/AgCl, 3 M KCl, respectively) (hnu - DeltaE(red)) is 1.33 eV, a large value which probably relates to the significant changes in distances and angles for the Ru-N-O moiety upon reduction. UV-vis absorptions, IR frequencies, and redox potentials are solvent-dependent. Controlled potential reduction (of NO(+)) and oxidation (of Ru(II) associated with the dicyano-chromophore) of I afford stable species, [NCRu(II)(py)(4)(CN)Ru(py)(4)NO](2+) (I(red)) and [NCRu(III)(py)(4)(...Continue Reading

References

Feb 24, 2001·Inorganic Chemistry·P V BernhardtM Martinez
Feb 24, 2001·Inorganic Chemistry·B R McGarveyD W Franco
Oct 24, 2001·Inorganic Chemistry·Simone da S. S. BorgesDouglas W. Franco
Oct 24, 2001·Inorganic Chemistry·Paula ForlanoJosé A. Olabe

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Citations

Mar 6, 2013·Inorganic Chemistry·German E PieslingerLuis M Baraldo
Nov 3, 2017·Dalton Transactions : an International Journal of Inorganic Chemistry·Paola S OviedoLuis M Baraldo
Jan 1, 2014·Angewandte Chemie·German E PieslingerLuis M Baraldo
May 8, 2010·Dalton Transactions : an International Journal of Inorganic Chemistry·Goutam Kumar Lahiri, Wolfgang Kaim
May 15, 2012·Dalton Transactions : an International Journal of Inorganic Chemistry·Giovanni Finoto CaramoriElia Tfouni
Feb 24, 2018·Inorganic Chemistry·Alejandro CadranelJosé H Hodak
Jul 30, 2014·Inorganic Chemistry·German E PieslingerLuis M Baraldo

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