Free-energy studies reveal a possible mechanism for oxidation-dependent inhibition of MGL

Sci Rep. 2016 Aug 8:6:31046. doi: 10.1038/srep31046.

Abstract

The function of monoacylglycerol lipase (MGL), a key actor in the hydrolytic deactivation of the endocannabinoid 2-arachidonoyl-sn-glycerol (2AG), is tightly controlled by the cell's redox state: oxidative signals such as hydrogen peroxide suppress MGL activity in a reversible manner through sulfenylation of the peroxidatic cysteines, C201 and C208. Here, using as a starting point the crystal structures of human MGL (hMGL), we present evidence from molecular dynamics and metadynamics simulations along with high-resolution mass spectrometry studies indicating that sulfenylation of C201 and C208 alters the conformational equilibrium of the membrane-associated lid domain of MGL to favour closed conformations of the enzyme that do not permit the entry of substrate into the active site.

Publication types

  • Research Support, Non-U.S. Gov't

MeSH terms

  • Catalytic Domain
  • Cysteine / chemistry
  • Humans
  • Hydrogen Bonding
  • Hydrogen Peroxide / chemistry
  • Molecular Dynamics Simulation
  • Monoacylglycerol Lipases / chemistry*
  • Oxidation-Reduction
  • Protein Binding
  • Protein Processing, Post-Translational
  • Thermodynamics

Substances

  • Hydrogen Peroxide
  • Monoacylglycerol Lipases
  • Cysteine