A substrate-induced switch in the reaction mechanism of a thermophilic esterase: kinetic evidences and structural basis

J Biol Chem. 2004 Feb 20;279(8):6815-23. doi: 10.1074/jbc.M307738200. Epub 2003 Nov 15.

Abstract

The reaction mechanism of the esterase 2 (EST2) from Alicyclobacillus acidocaldarius was studied at the kinetic and structural level to shed light on the mechanism of activity and substrate specificity increase previously observed in its double mutant M211S/R215L. In particular, the values of kinetic constants (k1, k(-1), k2, and k3) along with activation energies (E1, E(-1), E2, and E3) were measured for wild type and mutant enzyme. The previously suggested substrate-induced switch in the reaction mechanism from kcat=k3 with a short acyl chain substrate (p-nitrophenyl hexanoate) to kcat=k2 with a long acyl chain substrate (p-nitrophenyl dodecanoate) was validated. The inhibition afforded by an irreversible inhibitor (1-hexadecanesulfonyl chloride), structurally related to p-nitrophenyl dodecanoate, was studied by kinetic analysis. Moreover the three-dimensional structure of the double mutant bound to this inhibitor was determined, providing essential information on the enzyme mechanism. In fact, structural analysis explained the observed substrate-induced switch because of an inversion in the binding mode of the long acyl chain derivatives with respect to the acyl- and alcohol-binding sites.

Publication types

  • Research Support, Non-U.S. Gov't

MeSH terms

  • Alcohols / chemistry
  • Bacteria / enzymology*
  • Binding Sites
  • Caproates / chemistry
  • Carboxylic Ester Hydrolases / chemistry*
  • Catalysis
  • Crystallography, X-Ray
  • Dose-Response Relationship, Drug
  • Kinetics
  • Laurates / chemistry
  • Models, Chemical
  • Models, Molecular
  • Mutation
  • Nitrobenzenes / chemistry
  • Protein Binding
  • Substrate Specificity
  • Sulfones / pharmacology
  • Temperature
  • Time Factors

Substances

  • 1-hexadecanesulfonyl chloride
  • 4-nitrophenyl dodecanoate
  • 4-nitrophenyl hexanoate
  • Alcohols
  • Caproates
  • Laurates
  • Nitrobenzenes
  • Sulfones
  • Carboxylic Ester Hydrolases

Associated data

  • PDB/1QZ3