Chemoenzymatic synthesis of C-4'-spiro-oxetanoribonucleosides

J Org Chem. 2014 Sep 19;79(18):8516-21. doi: 10.1021/jo501655j. Epub 2014 Sep 8.

Abstract

Novozyme-435-mediated diastereoselective deacylation of one of the two diastereotopic acyloxymethyl groups in 5-O-acyl-4-C-acyloxymethyl-3-O-benzyl-1,2-O-isopropylidene-α-D-ribofuranose has been achieved in quantitative yield. The exclusive selectivity of the lipase for the 5-O-acyl over the 4-C-acyloxymethyl group in the substrate was confirmed by chemical transformation of enzymatically monodeacetylated compound to 1,2-O-isopropylidene-C-4-spiro-oxetanoribofuranose. Further, the selective biocatalytic deacylation methodology has been utilized for the efficient synthesis of C-4'-spiro-oxetanoribonucleosides of uracil (U) and thymine (T) in 37 and 45% overall yields, respectively.

Publication types

  • Research Support, Non-U.S. Gov't

MeSH terms

  • Molecular Structure
  • Monosaccharides / chemical synthesis*
  • Monosaccharides / chemistry
  • Ribonucleosides / chemical synthesis*
  • Ribonucleosides / chemistry
  • Spiro Compounds / chemical synthesis*
  • Spiro Compounds / chemistry
  • Stereoisomerism
  • Thymine / chemistry*
  • Uracil / chemistry*

Substances

  • 5-O-acyl-4-C-acyloxymethyl-3-O-benzyl-1,2-O-isopropylidene-alpha-D-ribofuranose
  • Monosaccharides
  • Ribonucleosides
  • Spiro Compounds
  • Uracil
  • Thymine