A water molecule in the stereospecificity pocket of Candida antarctica lipase B enhances enantioselectivity towards pentan-2-ol

Chembiochem. 2007 Apr 16;8(6):662-7. doi: 10.1002/cbic.200600479.

Abstract

The effect of water activity on enzyme-catalyzed enantioselective transesterification was studied by using a solid/gas reactor. The experimental results were compared with predictions from molecular modelling. The system studied was the esterification of pentan-2-ol with methylpropanoate as acyl donor and lipase B from Candida antarctica as catalyst. The data showed a pronounced water-activity effect on both reaction rate and enantioselectivity. The enantioselectivity increased from 100, at water activity close to zero, to a maximum of 320, at a water activity of 0.2. Molecular modelling revealed how a water molecule could bind in the active site and obstruct the binding of the slowly reacting enantiomer. Measurements of enantioselectivity at different water-activity values and temperatures showed that the water molecule had a high affinity for the stereospecificity pocket of the active site with a binding energy of 9 kJ mol-1, and that it lost all its degrees of rotation, corresponding to an entropic energy of 37 J mol-1 K-1.

MeSH terms

  • Acylation
  • Adsorption
  • Binding Sites
  • Bioreactors
  • Calibration
  • Candida / enzymology*
  • Catalysis
  • Fungal Proteins
  • Hydrolysis
  • Linear Models
  • Lipase / chemistry
  • Lipase / metabolism*
  • Models, Chemical
  • Models, Molecular
  • Pentanols / chemistry
  • Pentanols / metabolism*
  • Stereoisomerism
  • Substrate Specificity
  • Thermodynamics
  • Water / chemistry*

Substances

  • Fungal Proteins
  • Pentanols
  • Water
  • Lipase
  • lipase B, Candida antarctica