Enzymatic transition states, transition-state analogs, dynamics, thermodynamics, and lifetimes

Annu Rev Biochem. 2011:80:703-32. doi: 10.1146/annurev-biochem-061809-100742.

Abstract

Experimental analysis of enzymatic transition-state structures uses kinetic isotope effects (KIEs) to report on bonding and geometry differences between reactants and the transition state. Computational correlation of experimental values with chemical models permits three-dimensional geometric and electrostatic assignment of transition states formed at enzymatic catalytic sites. The combination of experimental and computational access to transition-state information permits (a) the design of transition-state analogs as powerful enzymatic inhibitors, (b) exploration of protein features linked to transition-state structure, (c) analysis of ensemble atomic motions involved in achieving the transition state, (d) transition-state lifetimes, and (e) separation of ground-state (Michaelis complexes) from transition-state effects. Transition-state analogs with picomolar dissociation constants have been achieved for several enzymatic targets. Transition states of closely related isozymes indicate that the protein's dynamic architecture is linked to transition-state structure. Fast dynamic motions in catalytic sites are linked to transition-state generation. Enzymatic transition states have lifetimes of femtoseconds, the lifetime of bond vibrations. Binding isotope effects (BIEs) reveal relative reactant and transition-state analog binding distortion for comparison with actual transition states.

Publication types

  • Research Support, N.I.H., Extramural
  • Review

MeSH terms

  • Animals
  • Drug Design
  • Enzyme Inhibitors / chemistry
  • Enzyme Inhibitors / metabolism
  • Enzymes / chemistry*
  • Enzymes / metabolism*
  • Humans
  • Isotopes / chemistry
  • Kinetics
  • Models, Molecular
  • Molecular Structure
  • Nucleosides / chemistry
  • Protein Conformation*
  • Static Electricity
  • Thermodynamics

Substances

  • Enzyme Inhibitors
  • Enzymes
  • Isotopes
  • Nucleosides