Sepetiba Bay, a key estuarine ecosystem in southeastern Brazil, faces significant metal inputs, with a differential pollution gradient from the bay's entrance to inner areas, raising environmental and public health concerns. This study assessed metal levels in fresh and cooked samples of highly consumed Charu mussels (Mytella charruana) from three bay areas, one near the bay entrance (P1), with higher water renewal rates, one in the northern bay area (P2) and one the eastern bay (P3), presenting lower water renewal rates. Variations in metal and metalloid concentrations across sites were observed, with P3 exhibiting higher levels in fresh mussels for most elements, except for As, which was higher at P2 (0.35 ± 0.45 mg kg−1). Cooked samples demonstrated similar trends for Cu (1.30 ± 0.39 mg kg−1), Ni (0.28 ± 0.20 mg kg−1), and V (0.75 ± 0.28 mg/kg−1), indicating that cooking in contaminanted estuary water does not significantly reduce contamination. Significant differences were detected for Ni, Cd (0.014 ± 0.008 mg kg−1), Zn (14.28 ± 2.50 mg kg−1), and V at P1, which were significantly higher than at P3. Significant Fe (246 ± 68 mg kg−1), Al (109 ± 33 mg kg−1), and Mn increases were observed from P1 to P3. Mussels sampled from P3, near an abandoned military area and urban center, exhibited high Fe and Al levels, attributed to both natural processes and industrial activities. Metal concentrations in Charu mussels often exceeded regulatory limits set by Brazilian, North American, and European agencies. Calculated Se molar ratios indicate that while Se can mitigate Hg toxicity, high Hg levels in Sepetiba Bay's Charu mussels still pose significant health risks. Similarly, high levels of Ag, Cd, and Pb suggest ineffective Se protection. However, Se appears effective against As toxicity. The Health Benefit Value of Selenium (HBVSe) indicate Se's overall protective benefits against Hg toxicity. Higher HBVSe values in cooked mussels at P1 and P2 suggest that cooking increases Se bioavailability. However, raw mussels at P3 had higher HBVSe values than cooked ones, highlighting the need for site-specific assessments. Calculated Hazard Indices indicate general high health risks from mussel consumption, and As levels in Charu mussels indicate high carcinogenic risks. These findings emphasize the need for comprehensive Charu mussel monitoring and environmental management efforts at Sepetiba Bay.
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