Structural and biochemical evidence for a boat-like transition state in beta-mannosidases

Nat Chem Biol. 2008 May;4(5):306-12. doi: 10.1038/nchembio.81.

Abstract

Enzyme inhibition through mimicry of the transition state is a major area for the design of new therapeutic agents. Emerging evidence suggests that many retaining glycosidases that are active on alpha- or beta-mannosides harness unusual B2,5 (boat) transition states. Here we present the analysis of 25 putative beta-mannosidase inhibitors, whose Ki values range from nanomolar to millimolar, on the Bacteroides thetaiotaomicron beta-mannosidase BtMan2A. B2,5 or closely related conformations were observed for all tightly binding compounds. Subsequent linear free energy relationships that correlate log Ki with log Km/kcat for a series of active center variants highlight aryl-substituted mannoimidazoles as powerful transition state mimics in which the binding energy of the aryl group enhances both binding and the degree of transition state mimicry. Support for a B2,5 transition state during enzymatic beta-mannosidase hydrolysis should also facilitate the design and exploitation of transition state mimics for the inhibition of retaining alpha-mannosidases--an area that is emerging for anticancer therapeutics.

Publication types

  • Research Support, Non-U.S. Gov't

MeSH terms

  • Enzyme Inhibitors / chemistry
  • Enzyme Inhibitors / pharmacology
  • Hydrolysis
  • Molecular Mimicry
  • Protein Conformation
  • beta-Mannosidase / antagonists & inhibitors
  • beta-Mannosidase / chemistry*
  • beta-Mannosidase / metabolism

Substances

  • Enzyme Inhibitors
  • beta-Mannosidase

Associated data

  • PDB/2VGU
  • PDB/2VJX
  • PDB/2VL4
  • PDB/2VMF
  • PDB/2VO5
  • PDB/2VOT
  • PDB/2VQT
  • PDB/2VR4