Variability in urinary biomarkers of human exposure to polycyclic aromatic hydrocarbons and its association with oxidative stress

Polycyclic aromatic hydrocarbons (PAHs) are ubiquitous environmental pollutants. Urinary concentrations of mono-hydroxylated metabolites of PAHs (OH-PAHs) have been used as biomarkers of these chemicals' exposure in humans. Little is known, however, with regard to intra- and inter-individual variability in OH-PAH concentrations and their association with oxidative stress. We conducted a longitudinal study of measurement of urinary concentrations of 15 OH-PAHs and 7 oxidative stress biomarkers (OSBs) of DNA damage [8-hydroxy-2'-deoxyguanosine (8-OHdG)], lipid [malondialdehyde (MDA) and F-2-isoprostanes (PGF(2 alpha))] and protein [o,o'-dityrosine (diY)] peroxidation in 19 individuals for 44 consecutive days. Metabolites of naphthalene (OHNap), fluorene (OHFlu), phenanthrene (OHPhe), and pyrene (OHPyr) were found in >70% of 515 urine samples analyzed, at sum concentrations (Sigma OH-PAH) measured in the range of 0.46-60 ng/mL. After adjusting for creatinine, OHNap and Sigma OH-PAH concentrations exhibited moderate predictability, with intra-class correlation coefficients (ICCs) ranging from 0.359 to 0.760. However, ICC values were low (0.001-0.494) for OHFlu, OHPhe, and OHPyr, which suggested poor predictability for these PAH metabolites. Linear mixed-effects analysis revealed that an unit increase in Sigma OH-PAH concentration corresponded to 4.5%, 5.3%, 20%, and 21% increase in respective urinary 8-OHdG, MDA, GF(2 alpha), and diY concentrations, suggesting an association with oxidative damage to DNA, lipids, and proteins. The daily intakes of PAHs, calculated from urinary concentrations of OH-PAHs, were 10- to 100-fold below the current reference doses. This study provides valuable information to design sampling strategies in biomonitoring studies and in assigning exposure classifications of PAHs in epidemiologic studies.

Automated summary

The study found that metabolites of polycyclic aromatic hydrocarbons (PAHs) were widely present in urine, with significant inter-individual variability in some metabolites' concentrations, showing association with oxidative stress. Linear mixed-effects analysis revealed a positive correlation between OH-PAH concentrations and oxidative damage to DNA, lipids, and proteins.