Efficient synthesis of NK(1) receptor antagonist aprepitant using a crystallization-induced diastereoselective transformation

J Am Chem Soc. 2003 Feb 26;125(8):2129-35. doi: 10.1021/ja027458g.

Abstract

An efficient stereoselective synthesis of the orally active NK(1) receptor antagonist Aprepitant is described. A direct condensation of N-benzyl ethanolamine with glyoxylic acid yielded a 2-hydroxy-1,4-oxazin-3-one which was activated as the corresponding trifluoroacetate. A Lewis acid mediated coupling with enantiopure (R)-1-(3,5-bis(trifluoromethyl)phenyl)ethan-1-ol afforded a 1:1 mixture of acetal diastereomers which was converted into a single isomer via a novel crystallization-induced asymmetric transformation. The resulting 1,4-oxazin-3-one was converted via a unique and highly stereoselective one-pot process to the desired alpha-(fluorophenyl)morpholine derivative. Interesting and unexpected [1,2]-Wittig and [1,3]-sigmatropic rearrangements were identified during the optimization of these key steps. In the final step, a triazolinone side chain was appended to the morpholine core. The targeted clinical candidate was thus obtained in 55% overall yield over the longest linear sequence.

MeSH terms

  • Aprepitant
  • Crystallography, X-Ray
  • Lactams / chemical synthesis
  • Lactams / chemistry
  • Molecular Structure
  • Morpholines / chemical synthesis*
  • Morpholines / chemistry
  • Neurokinin-1 Receptor Antagonists*
  • Oxazines / chemistry
  • Stereoisomerism

Substances

  • Lactams
  • Morpholines
  • Neurokinin-1 Receptor Antagonists
  • Oxazines
  • Aprepitant