Brassica juncea 3-hydroxy-3-methylglutaryl (HMG)-CoA synthase 1: expression and characterization of recombinant wild-type and mutant enzymes

Biochem J. 2004 Nov 1;383(Pt. 3):517-27. doi: 10.1042/BJ20040721.

Abstract

3-hydroxy-3-methylglutaryl (HMG)-CoA synthase (HMGS; EC 2.3.3.10) is the second enzyme in the cytoplasmic mevalonate pathway of isoprenoid biosynthesis, and catalyses the condensation of acetyl-CoA with acetoacetyl-CoA (AcAc-CoA) to yield S-HMG-CoA. In this study, we have first characterized in detail a plant HMGS, Brassica juncea HMGS1 (BjHMGS1), as a His6-tagged protein from Escherichia coli. Native gel electrophoresis analysis showed that the enzyme behaves as a homodimer with a calculated mass of 105.8 kDa. It is activated by 5 mM dithioerythreitol and is inhibited by F-244 which is specific for HMGS enzymes. It has a pH optimum of 8.5 and a temperature optimum of 35 degrees C, with an energy of activation of 62.5 J x mol(-1). Unlike cytosolic HMGS from chicken and cockroach, cations like Mg2+, Mn2+, Zn2+ and Co2+ did not stimulate His6-BjHMGS1 activity in vitro; instead all except Mg2+ were inhibitory. His6-BjHMGS1 has an apparent K(m-acetyl-CoA) of 43 microM and a V(max) of 0.47 micromol x mg(-1) x min(-1), and was inhibited by one of the substrates (AcAc-CoA) and by both products (HMG-CoA and HS-CoA). Site-directed mutagenesis of conserved amino acid residues in BjHMGS1 revealed that substitutions R157A, H188N and C212S resulted in a decreased V(max), indicating some involvement of these residues in catalytic capacity. Unlike His6-BjHMGS1 and its soluble purified mutant derivatives, the H188N mutant did not display substrate inhibition by AcAc-CoA. Substitution S359A resulted in a 10-fold increased specific activity. Based on these kinetic analyses, we generated a novel double mutation H188N/S359A, which resulted in a 10-fold increased specific activity, but still lacking inhibition by AcAc-CoA, strongly suggesting that His-188 is involved in conferring substrate inhibition on His6-BjHMGS1. Substitution of an aminoacyl residue resulting in loss of substrate inhibition has never been previously reported for any HMGS.

Publication types

  • Comparative Study
  • Research Support, Non-U.S. Gov't

MeSH terms

  • Acetyl-CoA Hydrolase / metabolism
  • Amino Acid Sequence
  • Animals
  • Arabidopsis Proteins / chemistry
  • Arginine / genetics
  • Avian Proteins / chemistry
  • Cations / metabolism
  • Chickens / genetics
  • Circular Dichroism / methods
  • Cockroaches / genetics
  • Fatty Acids, Unsaturated / metabolism
  • Gene Expression Regulation, Enzymologic / genetics
  • Histidine / biosynthesis
  • Histidine / chemistry
  • Histidine / metabolism
  • Humans
  • Hydrogen-Ion Concentration
  • Hydroxymethylglutaryl-CoA Synthase / biosynthesis
  • Hydroxymethylglutaryl-CoA Synthase / chemistry
  • Hydroxymethylglutaryl-CoA Synthase / genetics*
  • Hydroxymethylglutaryl-CoA Synthase / metabolism
  • Insect Proteins / chemistry
  • Kinetics
  • Lactones / metabolism
  • Mice
  • Molecular Sequence Data
  • Molecular Weight
  • Mustard Plant / enzymology*
  • Mutation / genetics
  • Plant Proteins / chemistry
  • Plant Proteins / genetics
  • Recombinant Proteins / metabolism
  • Schizosaccharomyces pombe Proteins / chemistry
  • Sequence Alignment / methods
  • Temperature

Substances

  • Arabidopsis Proteins
  • Avian Proteins
  • Cations
  • Fatty Acids, Unsaturated
  • Insect Proteins
  • Lactones
  • Plant Proteins
  • Recombinant Proteins
  • Schizosaccharomyces pombe Proteins
  • antibiotic 1233A
  • Histidine
  • Arginine
  • Hydroxymethylglutaryl-CoA Synthase
  • Acetyl-CoA Hydrolase