Advancing the Mechanistic Understanding of an Enantioselective Palladium-Catalyzed Alkene Difunctionalization Reaction.

The mechanism of an enantioselective palladium-catalyzed alkene difunctionalization reaction has been investigated. Kinetic analysis provides evidence of turnover-limiting attack of a proposed quinone methide intermediate with MeOH and suggests that copper is involved in productive product formation...

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Published in:Journal of the American Chemical Society Vol. 132; no. 49; pp. 17471 - 17483
Main Authors: Jensen, Katrina H., Webb, Jonathan D., Sigman, Matthew S.
Format: Article
Published: American Chemical Society 12/15/2010
Subjects:
Online Access:View this record in EBSCOhost
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      dt: 12/15/2010
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      pub: American Chemical Society
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        10.1021/ja108106h
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        atl: Advancing the Mechanistic Understanding of an Enantioselective Palladium-Catalyzed Alkene Difunctionalization Reaction.
      aug:
        au:
          Jensen, Katrina H.
          Webb, Jonathan D.
          Sigman, Matthew S.
        affil:
          Departments of Chemistry, University of Utah, 315 South 1400 East, Salt Lake City, Utah 84112, United States
          Queen's University, 90 Bader Lane, Kingston, Ontario K7L 3N6, Canada
      su:
        Enantioselective catalysis
        Ligands (Chemistry)
        Substrates (Materials science)
        Quantum perturbations
        Biocomplexity
        Palladium catalysts
        Alkenes
      sug:
        subj:
          Enantioselective catalysis
          Ligands (Chemistry)
          Substrates (Materials science)
          Quantum perturbations
          Biocomplexity
          Palladium catalysts
          Alkenes
      ab: The mechanism of an enantioselective palladium-catalyzed alkene difunctionalization reaction has been investigated. Kinetic analysis provides evidence of turnover-limiting attack of a proposed quinone methide intermediate with MeOH and suggests that copper is involved in productive product formation, not just catalyst turnover. Through examination of substrate electronic effects, a Jaffé relationship was observed correlating rate to electronic perturbation at two positions of the substrate. Ligand effects were evaluated to provide evidence of rapid ligand exchange between palladium and copper as well as a correlation between ligand electronic nature and enantioselectivity.
      pubtype: Academic Journal
      doctype: Article
      src: R
    language: English
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