Carbon-carbon bond cleavage in activation of the prodrug nabumetone

Drug Metab Dispos. 2014 May;42(5):828-38. doi: 10.1124/dmd.114.056903. Epub 2014 Feb 28.

Abstract

Carbon-carbon bond cleavage reactions are catalyzed by, among others, lanosterol 14-demethylase (CYP51), cholesterol side-chain cleavage enzyme (CYP11), sterol 17β-lyase (CYP17), and aromatase (CYP19). Because of the high substrate specificities of these enzymes and the complex nature of their substrates, these reactions have been difficult to characterize. A CYP1A2-catalyzed carbon-carbon bond cleavage reaction is required for conversion of the prodrug nabumetone to its active form, 6-methoxy-2-naphthylacetic acid (6-MNA). Despite worldwide use of nabumetone as an anti-inflammatory agent, the mechanism of its carbon-carbon bond cleavage reaction remains obscure. With the help of authentic synthetic standards, we report here that the reaction involves 3-hydroxylation, carbon-carbon cleavage to the aldehyde, and oxidation of the aldehyde to the acid, all catalyzed by CYP1A2 or, less effectively, by other P450 enzymes. The data indicate that the carbon-carbon bond cleavage is mediated by the ferric peroxo anion rather than the ferryl species in the P450 catalytic cycle. CYP1A2 also catalyzes O-demethylation and alcohol to ketone transformations of nabumetone and its analogs.

Publication types

  • Research Support, N.I.H., Extramural
  • Research Support, Non-U.S. Gov't

MeSH terms

  • Biocatalysis
  • Biotransformation
  • Butanones / metabolism*
  • Chromatography, High Pressure Liquid
  • Cyclooxygenase 2 Inhibitors / metabolism*
  • Cytochrome P-450 CYP1A2 / genetics
  • Cytochrome P-450 CYP1A2 / metabolism*
  • Escherichia coli / genetics
  • Humans
  • In Vitro Techniques
  • Microsomes / enzymology
  • Microsomes / metabolism
  • Nabumetone
  • Naphthaleneacetic Acids / metabolism*
  • Oxidation-Reduction
  • Prodrugs / metabolism*
  • Substrate Specificity
  • Transfection

Substances

  • Butanones
  • Cyclooxygenase 2 Inhibitors
  • Naphthaleneacetic Acids
  • Prodrugs
  • 6-methoxy-2-naphthylacetic acid
  • CYP1A2 protein, human
  • Cytochrome P-450 CYP1A2
  • Nabumetone