Causation in a Cascade: The Origins of Selectivities in Intramolecular Nitrone Cycloadditions.

The factors controlling chemo-, regio-, and stereoselectivity in a cascade of reactions starting from a bis(cyanoalkenyl)oxime and proceeding via nitrone cyclo- additions have been unraveled through a series of density functional theory calculations with several different functionals. Both kinetic a...

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Publicado en:Journal of the American Chemical Society Vol. 134; no. 29; pp. 12010 - 12016
Autores principales: Krenske, Elizabeth H., Agopcan, Sesil, Aviyente, Viktorya, Houk, K. N., Johnson, Brian A., Holmes, Andrew B.
Formato: Artículo
Publicado: American Chemical Society 7/25/2012
Materias:
Acceso en línea:Ver este registro en EBSCOhost
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        atl: Causation in a Cascade: The Origins of Selectivities in Intramolecular Nitrone Cycloadditions.
      aug:
        au:
          Krenske, Elizabeth H.
          Agopcan, Sesil
          Aviyente, Viktorya
          Houk, K. N.
          Johnson, Brian A.
          Holmes, Andrew B.
        affil:
          School of Chemistry, University of Melbourne, VIC 3010, Australia
          Australian Research Council Centre of Excellence for Free Radical Chemistry and Biotechnology
          Chemistry Department, Bogazici University, 34342 Bebek, Istanbul, Turkey
          Department of Chemistry and Biochemistry, University of California, Los Angeles, California 90095, United States
          CSIRO Materials Science and Engineering, Bag 10, Clayton South, VIC 3169, Australia
      su:
        Nitrones
        Ring formation (Chemistry)
        Regioselectivity (Chemistry)
        Density functionals
        Chemical models
        Thermodynamics
      sug:
        subj:
          Nitrones
          Ring formation (Chemistry)
          Regioselectivity (Chemistry)
          Density functionals
          Chemical models
          Thermodynamics
      ab: The factors controlling chemo-, regio-, and stereoselectivity in a cascade of reactions starting from a bis(cyanoalkenyl)oxime and proceeding via nitrone cyclo- additions have been unraveled through a series of density functional theory calculations with several different functionals. Both kinetic and thermodynamic control of the reaction cascade are important, depending upon the conditions. Kinetic control was analyzed by the distortion/interaction model and found to be dictated by differences in distortions of the cycloaddends in the transition states. A new mechanism competing with that originally proposed in the application of these reactions to the histrionicotoxin synthesis was discovered in these studies.
      pubtype: Academic Journal
      doctype: Article
      src: R
    language: English
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          year: 2012
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