Crystal structure of tert-butyldimethylsilyl-spiroaminooxathioledioxide-thymine (TSAO-T) in complex with HIV-1 reverse transcriptase (RT) redefines the elastic limits of the non-nucleoside inhibitor-binding pocket

J Med Chem. 2011 Apr 28;54(8):2727-37. doi: 10.1021/jm101536x. Epub 2011 Mar 29.

Abstract

tert-Butyldimethylsilyl-spiroaminooxathioledioxide (TSAO) compounds have an embedded thymidine-analogue backbone; however, TSAO compounds invoke non-nucleoside RT inhibitor (NNRTI) resistance mutations. Our crystal structure of RT:7 (TSAO-T) complex shows that 7 binds inside the NNRTI-binding pocket, assuming a "dragon" shape, and interacts extensively with almost all the pocket residues. The structure also explains the structure-activity relationships and resistance data for TSAO compounds. The binding of 7 causes hyper-expansion of the pocket and significant rearrangement of RT subdomains. This nonoptimal complex formation is apparently responsible (1) for the lower stability of a RT (p66/p51) dimer and (2) for the lower potency of 7 despite of its extensive interactions with RT. However, the HIV-1 RT:7 structure reveals novel design features such as (1) interactions with the conserved Tyr183 from the YMDD-motif and (2) a possible way for an NNRTI to reach the polymerase active site that may be exploited in designing new NNRTIs.

Publication types

  • Research Support, N.I.H., Extramural
  • Research Support, Non-U.S. Gov't

MeSH terms

  • Crystallography, X-Ray
  • Elasticity
  • HIV Reverse Transcriptase / antagonists & inhibitors*
  • Magnetic Resonance Spectroscopy
  • Models, Molecular
  • Molecular Structure
  • Reverse Transcriptase Inhibitors / pharmacology*
  • Spiro Compounds / chemistry*
  • Structure-Activity Relationship
  • Thymidine / analogs & derivatives*
  • Thymidine / chemistry
  • Uridine / analogs & derivatives

Substances

  • Reverse Transcriptase Inhibitors
  • Spiro Compounds
  • reverse transcriptase, Human immunodeficiency virus 1
  • HIV Reverse Transcriptase
  • Thymidine
  • TSAO-T
  • Uridine

Associated data

  • PDB/3QO9