Exploiting the π-Acceptor Properties of Carbene-Stabilized Phosphorus Centered Trications [LP] : Applications in Pt(II) Catalysis.

Reaction of tris(dimethylaminocyclopropenium) substituted phosphine 1 with KPtCl afforded the bench stable complex 3 which upon treatment with Ag[CBHCl] turned out to be an excellent catalyst for the transformation of a variety of ortho-biaryl substituted alkynes into polycyclic homo- and heteroaren...

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Publicado en:Journal of the American Chemical Society Vol. 134; no. 40; pp. 16753 - 16759
Autores principales: Carreras, Javier, Patil, Mahendra, Thiel, Walter, Alcarazo, Manuel
Formato: Artículo
Publicado: American Chemical Society 10/10/2012
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Acceso en línea:Ver este registro en EBSCOhost
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      dt: 10/10/2012
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      pub: American Chemical Society
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        82677134
        10.1021/ja306947m
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        atl: Exploiting the π-Acceptor Properties of Carbene-Stabilized Phosphorus Centered Trications [LP] : Applications in Pt(II) Catalysis.
      aug:
        au:
          Carreras, Javier
          Patil, Mahendra
          Thiel, Walter
          Alcarazo, Manuel
        affil: Max-Planck-Institut für Kohlenforschung, Kaiser-Wilhelm-Platz 1, D-45470 Mülheim an der Ruhr, Germany
      su:
        Carbenes
        Cations
        Phosphorus
        Density functionals
        Phosphorus compounds
        Surface chemistry
      sug:
        subj:
          Carbenes
          Cations
          Phosphorus
          Density functionals
          Phosphorus compounds
          Surface chemistry
      ab: Reaction of tris(dimethylaminocyclopropenium) substituted phosphine 1 with KPtCl afforded the bench stable complex 3 which upon treatment with Ag[CBHCl] turned out to be an excellent catalyst for the transformation of a variety of ortho-biaryl substituted alkynes into polycyclic homo- and heteroarenes of different size, shape, and curvature through a 6-endo-dig cyclization. This constitutes the first example ever reported of using a P-centered trication as ligand in catalysis. The strong π-acceptor character of 1 that derives from its three positive charges substantially increases the intrinsic π-acidity of Pt in complex 1·PtCl and dramatically enhances its ability to activate π-systems toward nucleophilic attack. As a consequence, a remarkable acceleration of the model transformation is observed when compared with other classical π-acceptor ligands such as P(OPh) or P(CF). Moreover, the employment of 1 as ligand also expands the scope of this reaction to previously inaccessible substitution patterns. Kinetic studies and deuterium labeling experiments as well as density functional theory (DFT) calculations were performed in order to explain these findings.
      pubtype: Academic Journal
      doctype: Article
      src: R
    language: English
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