Mechanism of xanthine oxidase catalyzed biotransformation of HMX under anaerobic conditions

Biochem Biophys Res Commun. 2003 Jun 27;306(2):509-15. doi: 10.1016/s0006-291x(03)01001-5.

Abstract

Enzyme catalyzed biotransformation of the energetic chemical octahydro-1,3,5,7-tetranitro-1,3,5,7-tetrazocine (HMX) is not known. The present study describes a xanthine oxidase (XO) catalyzed biotransformation of HMX to provide insight into the biodegradation pathway of this energetic chemical. The rates of biotransformation under aerobic and anaerobic conditions were 1.6+/-0.2 and 10.5+/-0.9 nmolh(-1)mgprotein(-1), respectively, indicating that anaerobic conditions favored the reaction. The biotransformation rate was about 6-fold higher using NADH as an electron-donor compared to xanthine. During the course of reaction, the products obtained were nitrite (NO(2)(-)), methylenedinitramine (MDNA), 4-nitro-2,4-diazabutanal (NDAB), formaldehyde (HCHO), nitrous oxide (N(2)O), formic acid (HCOOH), and ammonium (NH(4)(+)). The product distribution gave carbon and nitrogen mass-balances of 91% and 88%, respectively. A comparative study with native-, deflavo-, and desulfo-XO and the site-specific inhibition studies showed that HMX biotransformation occurred at the FAD-site of XO. Nitrite stoichiometry revealed that an initial single N-denitration step was sufficient for the spontaneous decomposition of HMX.

Publication types

  • Research Support, Non-U.S. Gov't
  • Research Support, U.S. Gov't, Non-P.H.S.

MeSH terms

  • Azocines / metabolism*
  • Carbon / chemistry
  • Dose-Response Relationship, Drug
  • Electrons
  • Formaldehyde / chemistry
  • Formates / chemistry
  • Heterocyclic Compounds, 1-Ring / metabolism*
  • Hydrocarbons
  • Hydrogen-Ion Concentration
  • Methane / analogs & derivatives*
  • Methane / chemistry
  • Models, Chemical
  • NAD / metabolism
  • Nitrites / metabolism
  • Nitrogen / chemistry
  • Nitrous Oxide / chemistry
  • Phenylenediamines / chemistry
  • Quaternary Ammonium Compounds / chemistry
  • Temperature
  • Time Factors
  • Xanthine Oxidase / metabolism*

Substances

  • Azocines
  • Formates
  • Heterocyclic Compounds, 1-Ring
  • Hydrocarbons
  • Nitrites
  • Phenylenediamines
  • Quaternary Ammonium Compounds
  • NAD
  • formic acid
  • Formaldehyde
  • carbene
  • Carbon
  • Xanthine Oxidase
  • Nitrous Oxide
  • octogen
  • Nitrogen
  • Methane
  • dinitramine