Exposure to chemical pollution can induce genetic and
epigenetic
alterations, developmental changes, and reproductive disorders, leading
to population declines in polluted environments. These effects are
triggered by chemical modifications of DNA nucleobases (DNA adducts)
and epigenetic dysregulation. However, linking DNA adducts to the
pollution load in situ remains challenging, and the
lack of evidence-based DNA adductome response to pollution hampers
the development and application of DNA adducts as biomarkers for environmental
health assessment. Here, we provide the first evidence for pollution
effects on the DNA modifications in wild populations of Baltic sentinel
species, the amphipod Monoporeia affinis. A workflow based on high-resolution mass spectrometry to screen
and characterize genomic DNA modifications was developed, and its
applicability was demonstrated by profiling DNA modifications in the
amphipods collected in areas with varying pollution loads. Then, the
correlations between adducts and the contaminants level (polycyclic
aromatic hydrocarbons (PAHs), trace metals, and pollution indices)
in the sediments at the collection sites were evaluated. A total of
119 putative adducts were detected, and some (5-me-dC, N6-me-dA, 8-oxo-dG, and dI) were structurally characterized. The DNA
adductome profiles, including epigenetic modifications, differed between
the animals collected in areas with high and low contaminant levels.
Furthermore, the correlations between the adducts and PAHs were similar
across the congeners, indicating possible additive effects. Also,
high-mass adducts had significantly more positive correlations with
PAHs than low-mass adducts. By contrast, correlations between the
DNA adducts and trace metals were stronger and more variable than
for PAHs, indicating metal-specific effects. These associations between
DNA adducts and environmental contaminants provide a new venue for
characterizing genome-wide exposure effects in wild populations and
apply DNA modifications in the effect-based assessment of chemical
pollution.