Preparative synthesis of drug metabolites using human cytochrome P450s 3A4, 2C9 and 1A2 with NADPH-P450 reductase expressed in Escherichia coli

J Ind Microbiol Biotechnol. 2005 Feb;32(2):67-74. doi: 10.1007/s10295-004-0202-1. Epub 2005 Mar 1.

Abstract

Three human cytochrome P450s, 3A4, 2C9 and 1A2, were each co-expressed with NADPH-P450 reductase in Escherichia coli and used in the preparative synthesis of drug metabolites. Low dissolved oxygen (DO) concentration (<1%) during expression was found to be critical for producing active P450s. Control of temperature, pH and glycerol supplementation in 10-L fermentations enhanced enzyme expression 31-86%. Additional improvements were obtained by altering media formulations, resulting in bicistronic expression levels of 890, 1,800 and 1,010 nmol/L for 3A4, 2C9 and 1A2, respectively. The P450 titers achieved in fermentors exceeded those in flask fermentations by 3- to 6-fold in this study and up to 10-fold when compared with previously reported literature. Intact cells and isolated membranes obtained from 10-L fermentations were used to establish an efficient bioconversion system for the generation of metabolites. To demonstrate the utility of this approach, known metabolites of the anabolic steroid testosterone, the anti-inflammatory agent diclofenac and the analgesic agent phenacetin, were generated using 3A4, 2C9 and 1A2, respectively. The reaction conditions were optimized for pH, temperature, DO concentration, use of co-solvent and glucose supplementation. Conversion yields of 29-93% were obtained from 1-L reactions, enabling isolation of 59 mg 6beta-hydroxytestosterone, 110 mg 4'-hydroxydiclofenac and 88 mg acetaminophen.

MeSH terms

  • Acetaminophen / metabolism
  • Aryl Hydrocarbon Hydroxylases / genetics*
  • Aryl Hydrocarbon Hydroxylases / metabolism
  • Biotransformation / genetics
  • Cloning, Molecular
  • Culture Media / chemistry
  • Cytochrome P-450 CYP1A2 / genetics*
  • Cytochrome P-450 CYP1A2 / metabolism
  • Cytochrome P-450 CYP2C9
  • Cytochrome P-450 CYP3A
  • Cytochrome P-450 Enzyme System / genetics*
  • Cytochrome P-450 Enzyme System / metabolism
  • Diclofenac / analogs & derivatives
  • Diclofenac / metabolism
  • Escherichia coli / genetics*
  • Escherichia coli / metabolism
  • Fermentation
  • Glycerol
  • Hydroxytestosterones / metabolism
  • NADPH-Ferrihemoprotein Reductase / genetics*
  • NADPH-Ferrihemoprotein Reductase / metabolism
  • Oxygen
  • Pharmaceutical Preparations / metabolism*
  • Phenacetin / metabolism
  • Recombinant Proteins / genetics
  • Recombinant Proteins / metabolism
  • Temperature
  • Testosterone / metabolism

Substances

  • Culture Media
  • Hydroxytestosterones
  • Pharmaceutical Preparations
  • Recombinant Proteins
  • Diclofenac
  • Acetaminophen
  • Testosterone
  • 6 beta-hydroxytestosterone
  • Cytochrome P-450 Enzyme System
  • CYP2C9 protein, human
  • Cytochrome P-450 CYP2C9
  • Aryl Hydrocarbon Hydroxylases
  • CYP3A protein, human
  • Cytochrome P-450 CYP1A2
  • Cytochrome P-450 CYP3A
  • NADPH-Ferrihemoprotein Reductase
  • Phenacetin
  • 4'-hydroxydiclofenac
  • Glycerol
  • Oxygen