Vinyl-ruthenium entities as markers for intramolecular electron transfer processes

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2011
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Inorganica Chimica Acta. 2011, 374(1), pp. 36-50. ISSN 0020-1693. Available under: doi: 10.1016/j.ica.2011.03.071
Zusammenfassung

The present account summarizes our work on mononuclear vinyl ruthenium complexes of the type RuCl(CHCHR′)(CO)(PR3)2L, divinyl-bridged diruthenium complexes {RuCl(CO)(PR3)2L}2(μ-CHCH-bridge-CHCH) and on heterobinuclear systems where only one of the two redox-active metal–organic moieties is of the vinyl ruthenium type. The favourable electrochemical properties of the {RuCl(CO)(PR3)2L(CHCH–) tag and the various spectroscopic handles offered by that unit provide detailed insights into the charge and spin delocalization over the {MCl(CO)(PR3)2L} and CHCHR′ constituents in their associated radical cations. They also offer a convenient means for measuring electronic coupling in the mixed-valent radical cations of the homo- and heterodinuclear vinyl-bridged complexes and, under favourable circumstances, on the rate of intramolecular electron transfer between the individual redox sites. Aspects of this work include examples of complexes showing time-dependent valence trapping, complexes aimed at delineating the efficiencies of through-space versus through-bond pathways for electron delocalization, complexes where electrostatic effects on the redox splitting ΔE1/2 dominate over those from the resonance contribution and systems that exhibit extensive charge and spin delocalization between two dislike endgroups despite their intrinsically different redox potentials.

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Fachgebiet (DDC)
540 Chemie
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Ruthenium, Vinyl complexes, Electrochemistry, Spectroelectrochemistry, Mixed-valent
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ISO 690MÜCKE, Philipp, Michael LINSEIS, Stanislav ZÁLIS, Rainer F. WINTER, 2011. Vinyl-ruthenium entities as markers for intramolecular electron transfer processes. In: Inorganica Chimica Acta. 2011, 374(1), pp. 36-50. ISSN 0020-1693. Available under: doi: 10.1016/j.ica.2011.03.071
BibTex
@article{Mucke2011Vinyl-13936,
  year={2011},
  doi={10.1016/j.ica.2011.03.071},
  title={Vinyl-ruthenium entities as markers for intramolecular electron transfer processes},
  number={1},
  volume={374},
  issn={0020-1693},
  journal={Inorganica Chimica Acta},
  pages={36--50},
  author={Mücke, Philipp and Linseis, Michael and Zális, Stanislav and Winter, Rainer F.}
}
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    <dcterms:abstract xml:lang="eng">The present account summarizes our work on mononuclear vinyl ruthenium complexes of the type RuCl(CHCHR′)(CO)(PR3)2L, divinyl-bridged diruthenium complexes {RuCl(CO)(PR3)2L}2(μ-CHCH-bridge-CHCH) and on heterobinuclear systems where only one of the two redox-active metal–organic moieties is of the vinyl ruthenium type. The favourable electrochemical properties of the {RuCl(CO)(PR3)2L(CHCH–) tag and the various spectroscopic handles offered by that unit provide detailed insights into the charge and spin delocalization over the {MCl(CO)(PR3)2L} and CHCHR′ constituents in their associated radical cations. They also offer a convenient means for measuring electronic coupling in the mixed-valent radical cations of the homo- and heterodinuclear vinyl-bridged complexes and, under favourable circumstances, on the rate of intramolecular electron transfer between the individual redox sites. Aspects of this work include examples of complexes showing time-dependent valence trapping, complexes aimed at delineating the efficiencies of through-space versus through-bond pathways for electron delocalization, complexes where electrostatic effects on the redox splitting ΔE1/2 dominate over those from the resonance contribution and systems that exhibit extensive charge and spin delocalization between two dislike endgroups despite their intrinsically different redox potentials.</dcterms:abstract>
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