Kirmse-Doyle- and Stevens-Type Rearrangements of Glutarate-Derived Oxonium Ylides

Chemistry. 2018 Mar 2;24(13):3209-3217. doi: 10.1002/chem.201704624. Epub 2018 Feb 5.

Abstract

A novel chemoenzymatic synthetic cascade enables the preparation of densely decorated tetrahydrofuran building blocks. Here, the lipase-catalyzed desymmetrization of 3-alkoxyglutarates renders highly enantioenriched carboxylic acid intermediates, whose subsequent activation and oxonium ylide rearrangement by means of rhodium or copper complexes furnishes functionalized O-heterocycles with excellent diastereoselectivity. The two-step protocol offers a streamlined and flexible synthesis of tetrahydrofuranones bearing different benzylic, allylic or allenylic side chains with full control over multiple stereogenic centers.

Keywords: chemoenzymatic; heterocycles; lipase; sigmatropic; transition metal catalysis.

MeSH terms

  • Carboxylic Acids / chemical synthesis
  • Carboxylic Acids / chemistry
  • Catalysis
  • Furans / chemical synthesis*
  • Furans / chemistry
  • Glutarates / chemistry*
  • Lipase / metabolism*
  • Molecular Structure
  • Oxazines / chemistry*
  • Stereoisomerism

Substances

  • Carboxylic Acids
  • Furans
  • Glutarates
  • Oxazines
  • Lipase