Analysis of phenoxyacetic acid herbicides as biomarkers in human urine using liquid chromatography/triple quadrupole mass spectrometry

Rapid Commun Mass Spectrom. 2008;22(2):143-50. doi: 10.1002/rcm.3348.

Abstract

Phenoxyacetic acids are widely used herbicides. The toxicity of phenoxyacetic acids is debated, but high-level exposure has been shown to be hepatotoxic as well as nephrotoxic in animal studies. An inter-species difference in toxic effects has been found, with dogs particularly susceptible. In this study a method using liquid chromatography/triple quadrupole mass spectrometry (LC/MS/MS) is described for the analysis of 4-chloro-2-methylphenoxyacetic acid (MCPA), and its metabolite 4-chloro-2-hydroxymethylphenoxyacetic acid (HMCPA), 2,4-dichlorophenoxyacetic acid (2,4-D), and 2,4,5-trichlorophenoxyacetic acid (2,4,5-T) in human urine. The urine samples were treated by acid hydrolysis to degrade possible conjugations. The sample preparation was performed using solid-phase extraction. Analysis was carried out using selected reaction monitoring (SRM) in the negative ion mode. Quantification of the phenoxyacetic acids was performed using [(2)H(3)]-labeled MCPA and 2,4-D as internal standards. The method was linear in the range 0.05-310 ng/mL urine and has a within-run precision of 2-5%. The between-run precision in lower concentration ranges was between 6-15% and between 2-8% in higher concentration ranges. The limit of detection was determined to 0.05 ng/mL. The metabolites in urine were found to be stable during storage at -20 degrees C. To validate the phenoxyacetic acids as biomarkers of exposure, the method was applied in a human experimental oral exposure to MCPA, 2,4-D and 2,4,5-T. Two healthy volunteers received 200 microg of each phenoxyacetic acid in a single oral dose followed by urine sampling for 72 h post-exposure. After exposure, between 90 and 101% of the dose was recovered in the urine. In the female subject, 23%, and in the male subject 17%, of MCPA was excreted as HMCPA.

Publication types

  • Research Support, Non-U.S. Gov't
  • Validation Study

MeSH terms

  • 2,4,5-Trichlorophenoxyacetic Acid / pharmacokinetics
  • 2,4,5-Trichlorophenoxyacetic Acid / urine
  • 2,4-Dichlorophenoxyacetic Acid / pharmacokinetics
  • 2,4-Dichlorophenoxyacetic Acid / urine
  • 2-Methyl-4-chlorophenoxyacetic Acid / analogs & derivatives
  • 2-Methyl-4-chlorophenoxyacetic Acid / pharmacokinetics
  • 2-Methyl-4-chlorophenoxyacetic Acid / urine*
  • Administration, Oral
  • Adult
  • Biomarkers / urine*
  • Chromatography, Liquid / methods*
  • Female
  • Herbicides / urine*
  • Humans
  • Male
  • Middle Aged
  • Reproducibility of Results
  • Spectrometry, Mass, Electrospray Ionization / methods*

Substances

  • Biomarkers
  • Herbicides
  • 2,4-Dichlorophenoxyacetic Acid
  • 2,4,5-Trichlorophenoxyacetic Acid
  • 2-Methyl-4-chlorophenoxyacetic Acid