Emerging and legacy contaminants across land-use gradients and the risk to aquatic ecosystems.

Information on potentially harmful emerging and legacy chemicals is essential to understand the risks to the environment and inform regulatory actions. The objective of this study was to assess the occurrence, concentration, and distribution of emerging and legacy contaminants across a gradient of land-use intensity and determine the risk posed to aquatic ecosystems. The land-use intensity gradient considered was: background/undeveloped < low-intensity agriculture < high-intensity agriculture < urban residential < urban industrial. Twenty-five sites were sampled for surface water, sediment, and soil. A total of 218 chemicals were analyzed: pesticides, per- and poly-fluoroalkyl substances (PFAS), polybrominated biphenyls and polybrominated diphenyl ethers (PBDEs), phthalates, and short-chain chlorinated paraffins (SCCPs). The risk posed by the analyzed chemicals to the aquatic environment was measured using hazard quotients (HQs), which were calculated by dividing the maximum measured environmental concentration by a predicted no-effect concentration for each chemical. A HQ > 1 was considered to indicate a high risk of adverse effects from the given chemical. A total of 68 chemicals were detected: 19 pesticides, 18 PFAS, 28 PBDEs, two phthalates, and SCCPs (as total SCCPs). There were no significant differences in the overall chemical composition between land uses. However, the insecticide bifenthrin, PFAS, PBDEs, and phthalates were more frequently found in samples from residential and/or industrial sites, suggesting urban land uses are hotspots and potential large-scale sources of these chemicals. Nineteen chemicals had a HQ > 1; most had a restricted spatial distribution limited to high-intensity agriculture and industrial sites in Melbourne. Bifenthrin and the perfluorooctanesulfonic acid (PFOS) had the highest HQs in residential and industrial sites, suggesting an increased risk to aquatic ecosystems in urban settings. The results of this study will enhance future research, predictive methods, and effective targeting of monitoring, and will help guide regulatory management actions and mitigation solutions.