Deuterium isotope effect on denitrosation and demethylation of N-nitrosodimethylamine by rat liver microsomes

Wade, D; Yang, CS; Metral, CJ; Roman, JM; Hrabie, JA; Riggs, CW; Anjo, T; Keefer, LK; Mico, BA

HERO ID

1665973

Reference Type

Journal Article

Year

1987

Language

English

PMID

3581074

HERO ID 1665973
In Press No
Year 1987
Title Deuterium isotope effect on denitrosation and demethylation of N-nitrosodimethylamine by rat liver microsomes
Authors Wade, D; Yang, CS; Metral, CJ; Roman, JM; Hrabie, JA; Riggs, CW; Anjo, T; Keefer, LK; Mico, BA
Journal Cancer Research
Volume 47
Issue 13
Page Numbers 3373-3377
Abstract In an attempt to elucidate the molecular basis for the decrease in rat liver carcinogenicity and DNA-alkylating ability that accompanies deuteration of N-nitrosodimethylamine (NDMA), NDMA and its fully deuterated analogue ([2H6]NDMA) were incubated with acetone-induced rat liver microsomes. Rates for the competing metabolic routes, denitrosation and demethylation, were determined from colorimetric data on nitrite and formaldehyde generation, respectively. The Vmax calculated for demethylation of NDMA was 7.9 nmol/min/mg, while that for denitrosation was 0.83 nmol/min/mg. Deuteration of NDMA did not significantly change the Vmax for either pathway, but it did increase the Km for demethylation from 0.06 to 0.3 mM. The Km for denitrosation was also increased from 0.06 to 0.3 mM on deuteration, as determined by incubating an equimolar mixture of amino-15N-labeled NDMA with [2H6]NDMA and measuring the methyl[15N]amine:[2H3]methylamine ratio by derivatization-gas chromatography-mass spectrometry. The fact that the Km values for denitrosation were so similar to those for demethylation suggested that the two pathways were catalyzed by the same enzyme. The isotope effects calculated from these data [VmaxH/VmaxD approximately 1 and (Vmax/Km)H/(Vmax/Km)D approximately 5] show that microsomal metabolism of NDMA is not significantly shifted from demethylation to denitrosation on deuteration of substrate and may indicate a low commitment to catalysis for the enzyme. The results are consistent with the view that the metabolism of NDMA is initiated by formation of an alpha-nitrosamino radical which either combines with a hydroxyl radical to form the alpha-hydroxynitrosamine as the initial product of the demethylation pathway or fragments to nitric oxide and N-methylformaldimine as the first products of denitrosation.
Pmid 3581074
Is Certified Translation No
Dupe Override No
Is Public Yes
Language Text English
Keyword Animals; Cytochrome P-450 CYP2E1; Deuterium; Dimethylnitrosamine/metabolism; Kinetics; Mass Spectrometry; Methylation; Microsomes, Liver/metabolism; Nitrates/metabolism; Oxidoreductases, N-Demethylating/metabolism; 62-75-9; 7782-39-0; EC 1.14.14.1; EC 1.5.-