In vitro and in vivo properties of therapeutic oligonucleotides containing non-chiral 3' and 5' thiophosphate linkages

Nucleic Acids Res. 2020 Jan 10;48(1):63-74. doi: 10.1093/nar/gkz1099.

Abstract

The introduction of non-bridging phosphorothioate (PS) linkages in oligonucleotides has been instrumental for the development of RNA therapeutics and antisense oligonucleotides. This modification offers significantly increased metabolic stability as well as improved pharmacokinetic properties. However, due to the chiral nature of the phosphorothioate, every PS group doubles the amount of possible stereoisomers. Thus PS oligonucleotides are generally obtained as an inseparable mixture of a multitude of diastereoisomeric compounds. Herein, we describe the introduction of non-chiral 3' thiophosphate linkages into antisense oligonucleotides and report their in vitro as well as in vivo activity. The obtained results are carefully investigated for the individual parameters contributing to antisense activity of 3' and 5' thiophosphate modified oligonucleotides (target binding, RNase H recruitment, nuclease stability). We conclude that nuclease stability is the major challenge for this approach. These results highlight the importance of selecting meaningful in vitro experiments particularly when examining hitherto unexplored chemical modifications.

Publication types

  • Research Support, Non-U.S. Gov't

MeSH terms

  • Animals
  • Apolipoprotein B-100 / antagonists & inhibitors
  • Apolipoprotein B-100 / genetics*
  • Apolipoprotein B-100 / metabolism
  • Cell Line, Tumor
  • Female
  • Humans
  • Kidney / cytology
  • Kidney / metabolism
  • Liver / cytology
  • Liver / metabolism
  • Lung / metabolism
  • Lung / pathology
  • Mice
  • Mice, Inbred C57BL
  • Oligonucleotides / chemical synthesis
  • Oligonucleotides / genetics*
  • Oligonucleotides / metabolism
  • Phosphates / chemistry*
  • Phosphates / metabolism
  • Phosphorothioate Oligonucleotides / chemical synthesis
  • Phosphorothioate Oligonucleotides / genetics*
  • Phosphorothioate Oligonucleotides / metabolism
  • RNA Stability
  • RNA, Long Noncoding / antagonists & inhibitors
  • RNA, Long Noncoding / genetics*
  • RNA, Long Noncoding / metabolism
  • Ribonuclease H / chemistry
  • Ribonuclease H / metabolism
  • Stereoisomerism

Substances

  • Apob protein, mouse
  • Apolipoprotein B-100
  • MALAT1 long non-coding RNA, human
  • Oligonucleotides
  • Phosphates
  • Phosphorothioate Oligonucleotides
  • RNA, Long Noncoding
  • locked nucleic acid
  • Ribonuclease H
  • thiophosphoric acid