Mechanism-based inactivation of cytochrome P450 2A6 and 2A13 by Rhinacanthus nasutus constituents

Drug Metab Pharmacokinet. 2014;29(1):75-82. doi: 10.2133/dmpk.dmpk-13-rg-048. Epub 2013 Jul 30.

Abstract

Human cytochrome P450 CYP2A6 and CYP2A13 catalyze nicotine metabolisms and mediate activation of tobacco-specific carcinogens including 4-(methylnitrosamino)-1-(3-pyridyl)-1-butanone (NNK) and 4-(methylnitrosamino)-1-(3-pyridyl)-1-butanol (NNAL). In this study, we found rhinacanthins A, B, and C isolated from Rhinacanthus nasutus potentially inhibited coumarin 7-hydroxylation mediated by reconstituted purified recombinant CYP2A6 and CYP2A13. Rhinacanthins A-C are mechanism-based inactivators of CYP2A6 and CYP2A13 as they cause concentration, time and NADPH-dependent inhibition. Among the three rhinacanthins, rhinacanthin-B possessed highest inhibitory potency against CYP2A13 with apparent KI and kinact of 0.16 µM and 0.1 min(-1), respectively, while values of 0.44 µM and 0.12 min(-1) were found against CYP2A6. Rhinacanthin-C had least inhibition potency, with apparent KI and kinact of 0.97 µM and 0.07 min(-1) for CYP2A6, respectively, and values of 1.68 µM and 0.05 min(-1) for CYP2A13. Rhinacanthin-A inhibited CYP2A6 and CYP2A13 with apparent KI values of 0.69 and 0.42 µM, respectively and apparent kinact of 0.18 and 0.06 min(-1), respectively. The inhibition of both enzymes by rhinacanthins A-C could not be prevented by addition of trapping agents or reversed by dialysis or potassium ferricyanide. These findings demonstrated that rhinacanthins A-C, which are 1,4-naphthoquinone derivatives, irreversibly inhibited CYP2A6 and CYP2A13 in a mechanism-based inhibition mode.

MeSH terms

  • Acanthaceae / chemistry*
  • Animals
  • Aryl Hydrocarbon Hydroxylases / antagonists & inhibitors*
  • Aryl Hydrocarbon Hydroxylases / chemistry
  • Coumarins / chemistry
  • Cytochrome P-450 CYP2A6
  • Humans
  • Hydroxylation
  • Kinetics
  • NADPH-Ferrihemoprotein Reductase / chemistry
  • Naphthoquinones / chemistry*
  • Plant Extracts / chemistry
  • Rats
  • Recombinant Proteins / chemistry

Substances

  • Coumarins
  • Naphthoquinones
  • Plant Extracts
  • Recombinant Proteins
  • rhinacanthin-A
  • rhinacanthin-B
  • rhinacanthin-C
  • coumarin
  • Aryl Hydrocarbon Hydroxylases
  • CYP2A13 protein, human
  • CYP2A6 protein, human
  • Cytochrome P-450 CYP2A6
  • NADPH-Ferrihemoprotein Reductase