Influence of Environmental Factors on the Fate of Legacy and Emerging Per- and Polyfluoroalkyl Substances along the Salinity/Turbidity Gradient of a Macrotidal Estuary

This study aimed at bridging knowledge gaps regarding the land-sea transport of per- and polyfluoroalkyl substances (PFASs) through riverine discharge into coastal waters. The present survey was conducted in the Gironde estuary (southwestern France) where PFASs were ubiquitously detected albeit at low levels. Emerging Sigma PFASs such as fluorotelomer sulfonates or polyfluoroalkyl phosphate diesters accounted for a relatively minor proportion of Sigma PFASs, while perfluorooctanesulfonate, perfluorohexanesulfonate, and perfluorohexanoate were the predominant congeners. Multiple linear regressions provided insights into the relative influence of factors controlling PFAS sediment levels. In that respect, the organic carbon fraction (strongly correlated to sediment grain size) appeared as a more important controlling factor than black carbon or distance from upstream sources for long-chain perfluoroalkyl acids. In the maximum turbidity zone (suspended solids up to 2600 mg L-1), the particle-associated fraction was almost consistently >50% for long-chain perfluoroalkyl carboxylates and sulfonates (>= C8 and >= C6, respectively). Empirical models of K-D partitioning coefficients were derived by integrating, for the first time, both particle-concentration and salting-out effects. These results represent significant progress toward the development of numerical transport models integrating both PFAS partitioning and 3D-hydrosedimentary dynamics, with a view to estimate PFAS mass budgets at the land-sea interface.