A GC/MS method for the quantitation of N-nitrosoproline and N-
acetyl-S-allylcysteine in human urine:
Application to a study of the effects of garlic consumption on nitrosation
Keary Cope
1
, Harold Seifried
2
, Rebecca Seifried
1,3
, John Milner
2,3
, Penny Kris-Etherton
2
,
and Earl H. Harrison
1
1
Phytonutrients Laboratory, USDA Human Nutrition Research Center, Beltsville, MD 20705
2
Nutritional Sciences Research Group, Division of Cancer Prevention, National Cancer Institute,
Rockville, MD 20892
3
Department of Nutritional Sciences Penn State University; University Park, PA 16802
Abstract
Biomarkers in urine can provide useful information about the bioactivation of chemical carcinogens
and can be used to investigate the chemoprotective properties of dietary nutrients. N-nitrosoproline
(NPRO) excretion has been used as an index for endogenous nitrosation. In vitro and animal studies
have reported that compounds in garlic may suppress nitrosation and inhibit carcinogenesis. We
present a new method for extraction and sensitive detection of both NPRO and N-acetyl-S-
allylcysteine from urine. The latter is a major metabolite of S-allyl cysteine which is abundant in
garlic. Urine was acidified and the organic acids extracted by reversed phase extraction (RP-SPE)
and use of a polymeric weak anion exchange (WAX-SPE) resin. NPRO was quantified by isotope
dilution gas chromatography-mass spectrometry using
13
C
5
NPRO and N-nitrosopipecolic acid
(NPIC) as internal standards. This method was used to analyze urine samples from a study that was
designed to test whether garlic supplementation inhibits NPRO synthesis. Using this method, 2.4 to
46 ng of NPRO per mL urine was detected. The method is straightforward, reliable and can be
performed with readily available GC/MS instruments. N-acetyl-S-allylcysteine was quantified in the
same fraction and detectable at levels of 4.1 to 176.4 ng per mL of urine. The results suggest that 3
to 5 grams of garlic supplements inhibited NPRO synthesis to an extent similar to a 0.5 g dose of
ascorbic acid or a commercial supplement of aged garlic extract. Urinary NPRO concentration was
inversely associated with the N-acetyl-S-allylcysteine concentration. It is possible that allyl sulfur
compounds found in garlic may inhibit nitrosation in humans. .
Keywords
biomarkers; allyl sulfur compounds; nitrosation; nutrition; cancer
© 2009 Elsevier Inc. All rights reserved.
Address correspondence to: Earl Harrison, Department of Human Nutrition, The Ohio State University, Columbus, OH 43210,
614-292-8189, Harrison.304@osu.edu.
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Author Manuscript
Anal Biochem. Author manuscript; available in PMC 2010 November 15.
Published in final edited form as:
Anal Biochem. 2009 November 15; 394(2): 243–248. doi:10.1016/j.ab.2009.07.035.
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