Dynamic spatiotemporal changes of per- and polyfluoroalkyl substances (PFAS) in soil and eggs of private gardens at different distances from a fluorochemical plant

Homegrown food serves as an important human exposure source of perand polyfluoroalkyl substances (PFAS), yet little is known about their spatiotemporal distribution within and among private gardens. This knowledge is essential for more accurate site -specific risk assessment, identification of new sources and evaluating the effectiveness of regulations. The present study evaluated spatiotemporal changes of legacy and emerging PFAS in surface soil from vegetable gardens (N = 78) and chicken enclosures (N = 102), as well as in homegrown eggs (N = 134) of private gardens, across the Province of Antwerp (Belgium). Hereby, the potential influence of the wind orientation and distance towards a major fluorochemical plant was examined. The & sum;short-chain PFAS and precursor concentrations were higher in vegetable garden soil (8.68 ng/g dry weight (dw)) compared to chicken enclosure soil (4.43 ng/g dw) and homegrown eggs (0.77 ng/g wet weight (ww)), while long -chain sulfonates and C-11_14 carboxylates showed the opposite trend. Short-term (2018/2019-2022) changes were mostly absent in vegetable garden soil, while changes in chicken enclosure soils oriented S -SW nearby (<4 km) the fluorochemical plant were characterized by a local, high -concentration plume. Moreover, soil from chicken enclosures oriented SE and remotely from the plant site was characterized by a widespread, diffuse but relatively lowconcentration plume. Long-term data (2010-2022) suggest that phaseout and regulatory measures have been effective, as PFOS concentrations nearby the fluorochemical plant in soil and eggs have declined from 25.8 to 2.86 ng/g dw and from 528 to 39.4 ng/g ww, respectively. However, PFOS and PFOA concentrations have remained largely stable within this timeframe in gardens remotely from the plant site, warranting further rapid regulation and remediation measures. Future monitoring efforts are needed to allow long-term comparison for multiple PFAS and better distinction from potential confounding variables, such as variable emission outputs and variability in wind patterns.