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Complexation Equilibria: The Chelate Effect01:19

Complexation Equilibria: The Chelate Effect

In complexation reactions, metal atoms or cations interact with ligands to form donor-acceptor adducts called metal complexes. Ligands that bind through one donor site are monodentate, ligands with two donor sites are bidentate, and those with more than two donor sites are polydentate ligands. For example, ethylene diamine is a bidentate ligand that binds through two nitrogen donor atoms, forming a five-membered ring. EDTA is a polydentate ligand that binds through four oxygen and two nitrogen...
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Introduction
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Aromatic Hydrocarbon Cations: Structural Overview01:18

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Cycloheptatriene is a neutral monocyclic unsaturated hydrocarbon that consists of an odd number of carbon atoms and an intervening sp3 carbon in the ring. The three double bonds in the ring correspond to 6 π electrons, which is a Huckel number, and therefore satisfies the criteria of 4n + 2 π electrons. However, the intervening sp3 carbon disrupts the continuous overlap of p orbitals. As a result, cycloheptatriene is not aromatic.
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Functionalized arene-ruthenium(II) complexes: dangling vs. tethering side chain.

Beatriz Lastra-Barreira1, Josefina Díez, Pascale Crochet

  • 1Laboratorio de Compuestos Organometálicos y Catálisis (Unidad Asociada al CSIC), Departamento de Química Orgánica e Inorgánica - IUQOEM, Universidad de Oviedo, C/Julián Clavería 8, E-33006 Oviedo, Spain.

Dalton Transactions (Cambridge, England : 2003)
|February 20, 2013
PubMed
Summary

Ruthenium complexes with phosphine or phosphite ligands show varied reactivity with silver hexafluoroantimonate. This leads to different dinuclear or tethered structures, explained by theoretical calculations.

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Area of Science:

  • Organometallic Chemistry
  • Coordination Chemistry
  • Synthetic Inorganic Chemistry

Background:

  • Ruthenium complexes are versatile catalysts and precursors in organic synthesis.
  • The influence of ligand type on the reactivity of ruthenium complexes is crucial for designing new synthetic routes.
  • Understanding chloride abstraction reactions is key to controlling the nuclearity and structure of metal complexes.

Purpose of the Study:

  • To investigate the reactivity of specific ruthenium(II) complexes with varying side chains towards chloride abstraction.
  • To elucidate the structural outcomes of reactions involving silver hexafluoroantimonate (AgSbF6) as a chloride abstractor.
  • To rationalize the observed differences in reactivity and product formation through theoretical analysis.

Main Methods:

  • Synthesis and characterization of ruthenium(II) complexes with η(6)-arene ligands bearing alcohol functionalities.
  • Reaction of ruthenium complexes with the chloride abstractor silver hexafluoroantimonate (AgSbF6).
  • Spectroscopic (NMR) and X-ray crystallographic analyses of the resulting products.
  • Computational studies (theoretical calculations) to explain reactivity differences.

Main Results:

  • The triphenylphosphite complex [RuCl2(η(6)-C6H5OCH2CH2OH)(P(OPh)3)] reacted with AgSbF6 to form a dinuclear dichloro-bridged species.
  • The triphenylphosphine analog [RuCl2(η(6)-C6H5OCH2CH2OH)(PPh3)] yielded a di-ruthenium derivative with a single chloride bridge.
  • Ruthenium complexes with a longer propyl alcohol chain [RuCl2(η(6)-C6H5CH2CH2CH2OH)(L)] cleanly formed tethered compounds where the alcohol oxygen coordinated to ruthenium.
  • Theoretical calculations provided insights into the factors governing the distinct reaction pathways.

Conclusions:

  • The nature of the phosphine/phosphite ligand and the length of the alcohol side chain significantly influence the outcome of chloride abstraction reactions.
  • The formation of dinuclear bridged species versus tethered complexes is dependent on subtle electronic and steric effects.
  • Computational modeling is a valuable tool for understanding and predicting the reactivity of organometallic complexes.