Optimized synthesis of phosphorothioate oligodeoxyribonucleotides substituted with a 5'-protected thiol function and a 3'-amino group

Nucleic Acids Res. 2000 Feb 1;28(3):818-25. doi: 10.1093/nar/28.3.818.

Abstract

A new deprotection procedure enables a medium scale preparation of phosphodiester and phosphor-othioate oligonucleotides substituted with a protected thiol function at their 5'-ends and an amino group at their 3'-ends in good yield (up to 72 OD units/micromol for a 19mer phosphorothioate). Syntheses of 3'-amino-substituted oligonucleotides were carried out on a modified support. A linker containing the thioacetyl moiety was manually coupled in two steps by first adding its phosphor-amidite derivative in the presence of tetrazole followed by either oxidation or sulfurization to afford the bis-derivatized oligonucleotide bound to the support. Deprotection was achieved by treating the fully protected oligonucleotide with a mixture of 2,2'-dithiodipyridine and concentrated aqueous ammonia in the presence of phenol and methanol. This proced-ure enables (i) cleavage of the oligonucleotide from the support, releasing the oligonucleotide with a free amino group at its 3'-end, (ii) deprotection of the phosphate groups and the amino functions of the nucleic bases, as well as (iii) transformation of the 5'-terminal S -acetyl function into a dithiopyridyl group. The bis-derivatized phosphorothioate oligomer was further substituted through a two-step procedure: first, the 3'-amino group was reacted with fluorescein isothiocyanate to yield a fluoresceinylated oligo-nucleotide; the 5'-dithio-pyridyl group was then -quantitatively reduced to give a free thiol group which was then substituted by reaction with an N alpha-bromoacetyl derivative of a signal peptide containing a KDEL sequence to afford a fluoresceinylated peptide-oligonucleotide conjugate.

Publication types

  • Research Support, Non-U.S. Gov't

MeSH terms

  • Amides / chemistry
  • Amines / chemistry
  • Amino Acid Sequence
  • Base Sequence
  • Chromatography, High Pressure Liquid
  • Disulfides / chemistry
  • Electrophoresis, Polyacrylamide Gel
  • Fluorescein-5-isothiocyanate / chemistry
  • Mass Spectrometry
  • Methanol / chemistry
  • Oligodeoxyribonucleotides / chemical synthesis*
  • Oligodeoxyribonucleotides / chemistry*
  • Oligodeoxyribonucleotides / genetics
  • Oligodeoxyribonucleotides / isolation & purification
  • Oligopeptides / chemistry
  • Oligopeptides / genetics
  • Oxidation-Reduction
  • Phenol / chemistry
  • Phosphates / chemistry
  • Phosphoramides
  • Phosphoric Acids / chemistry
  • Protein Sorting Signals*
  • Pyridines / chemistry
  • Sulfhydryl Compounds / chemistry
  • Tetrazoles / chemistry
  • Thionucleotides / chemical synthesis*
  • Thionucleotides / chemistry*
  • Thionucleotides / genetics

Substances

  • Amides
  • Amines
  • Disulfides
  • Oligodeoxyribonucleotides
  • Oligopeptides
  • Phosphates
  • Phosphoramides
  • Phosphoric Acids
  • Protein Sorting Signals
  • Pyridines
  • Sulfhydryl Compounds
  • Tetrazoles
  • Thionucleotides
  • lysyl-aspartyl-glutamyl-leucine
  • phosphoramide
  • 1H-tetrazole
  • Phenol
  • Fluorescein-5-isothiocyanate
  • Methanol