Distribution behavior and risk assessment of emerging perfluoroalkyl acids in multiple environmental media at Luoma Lake, East China

Perfluoroalkyl acids (PFAAs) are ubiquitous in various environments. This has caused great public concern, particularly in the shallow freshwater lake region, where the lake, rivers, and estuaries form a highly interconnected continuum. However, little is known about the environmental behaviors of PFAAs in the continuum. For the first time, a high-resolution monitoring framework covering the river-estuary-lake continuum of Luoma Lake was built, and the concentrations, sources, and environmental fates of PFAAs were identified and analyzed. The results revealed that the total concentration of PFAAs was at a moderate level in the water and at a high level in the sediment compared to global levels respectively. Perfluorooctanesulfonate (PFOS) was the most abundant PFAA in the continuum. In particular, the ∑PFAA concentration in the particle phase was much higher than that in the sediment phase. Distinct spatial heterogeneities were observed in the behaviors of distribution and the multiphase fate of PFAAs in the continuum, mainly driven by the turbulent mixing during transport, dilution of lake water, and spatial differences of hydrodynamic features and sedimentary properties among the sub-regions. Interestingly, the pH of the sediment and water had significant effects on the water-sediment portioning of PFAAs in contrasting ways. Furthermore, based on the composition of the sediments, four possible migration paths for PFAAs were deduced and the main sources of PFAAs were identified as sewage, domestic, and industrial effluents using the positive matrix factorization model. During the human health assessment, no risk was found under the median exposure scenario; however, under the high exposure scenario, PFAAs posed uncertain risks to human health, which cannot be ignored. This study provides basic information for simulating the fate and transport of PFAAs in the continuum and is significant for developing cost-effective control and remediation strategies in the near future.