Hemichelation, a Way To Stabilize Electron-Unsaturated Complexes: The Case of T-Shaped Pd and Pt Metallacycles.

A rational method of synthesis of stable neutral T-shaped 14 electron Pd and Pt complexes is proposed. It takes advantage of the ambiphilic character of the tricarbonyl(η-indenyl)chromium anion, of which the main property is to behave as a hemichelating ligand, that is a nonconventional heteroditopi...

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Publicado en:Journal of the American Chemical Society Vol. 135; no. 47; pp. 17839 - 17853
Autores principales: Werlé, Christophe, Bailly, Corinne, Karmazin-Brelot, Lydia, Le Goff, Xavier-Frédéric, Ricard, Louis, Djukic, Jean-Pierre
Formato: Artículo
Publicado: American Chemical Society 11/27/2013
Materias:
Acceso en línea:Ver este registro en EBSCOhost
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      dt: 11/27/2013
      vid: 135
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      pub: American Chemical Society
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        10.1021/ja4076327
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        atl: Hemichelation, a Way To Stabilize Electron-Unsaturated Complexes: The Case of T-Shaped Pd and Pt Metallacycles.
      aug:
        au:
          Werlé, Christophe
          Bailly, Corinne
          Karmazin-Brelot, Lydia
          Le Goff, Xavier-Frédéric
          Ricard, Louis
          Djukic, Jean-Pierre
        affil:
          Institut de Chimie de Strasbourg, Université de Strasbourg, CNRS, 4 rue Blaise Pascal, F-67000 Strasbourg, France
          Département de Chimie, Ecole Polytechnique, CNRS, Route de Saclay, F-91128 Palaiseau cedex, France
      su:
        Metallacycles
        Electron research
        Density functionals
        Ligands (Chemistry)
        Nuclear particle research
      sug:
        subj:
          Metallacycles
          Electron research
          Density functionals
          Ligands (Chemistry)
          Nuclear particle research
      ab: A rational method of synthesis of stable neutral T-shaped 14 electron Pd and Pt complexes is proposed. It takes advantage of the ambiphilic character of the tricarbonyl(η-indenyl)chromium anion, of which the main property is to behave as a hemichelating ligand, that is a nonconventional heteroditopic ligand capable of chelating a metal center by way of covalent and noncovalent bonding, thus preserving its unsaturated valence shell. The reaction of the in situ formed tricarbonyl(η-2-methylindenyl)chromium anion with a series of Pd and Pt metallacycles afforded new air-stable and persistent synfacial heterobimetallic complexes in which the metallacycle binds the indenyl fragment via its metal in an η fashion, leaving the fourth coordination site at the chelated metal virtually vacant. The structures of eight of these novel complexes are disclosed, and their bonding features are investigated by an array of theoretical methods based on the density functional theory (NBO, EDA, ETS-NOCV, AIM, NCI region analysis). Theory shows that the formation of these unusual structures of bimetallic synfacial η-indenyl-Pd/Pt complexes is driven thermodynamically by attractive Coulombic occlusion of the fourth vacant coordination site at Pd/Pt centers by the Cr(CO) moiety.
      pubtype: Academic Journal
      doctype: Article
      src: R
    language: English
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          year: 2013
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