Prediction of perfluoroalkyl acids (PFAAs) in homegrown eggs: Insights into abiotic and biotic factors affecting bioavailability and derivation of potential remediation measures.

Homegrown eggs from free-ranging laying hens often contain elevated concentrations of perfluoroalkyl acids (PFAAs). However, it is unclear which factors contribute to these relatively large exposure risk scenarios. Moreover, existing bioavailability and modeling concepts of conventional organic pollutants cannot be generalized to PFAAs due to their different physicochemical soil interactions. Therefore, there is an urgent need for empirical models, based on real-world data, to provide insights into how (a)biotic factors affect the bioavailability to eggs. To this end, 17 targeted analytes were analyzed in abiotic (i.e. rainwater, soil; both N = 101) matrices and homegrown eggs (N = 101), which were sampled in 101 private gardens across Flanders (Belgium) in 2019, 2021 and 2022. Various soil characteristics were measured to evaluate their role in affecting PFAA bioavailability to the eggs. Finally, PFAAs were measured in potential feed sources (i.e. homegrown vegetable and earthworm pools; respectively N = 49 and N = 34) of the laying hens to evaluate their contribution to the egg burden. Modeling suggested that soil was a major exposure source to laying hens, accounting for 16-55% of the total variation in egg concentrations for dominant PFAAs. Moreover, concentrations in vegetables and earthworms for PFBA and PFOS, respectively, were significantly positively related with corresponding egg concentrations. Predictive models based on soil concentrations, total organic carbon (TOC), pH, clay content and exchangeable cations were successfully developed for major PFAAs, providing possibilities for time- and cost-effective risk assessment of PFAAs in homegrown eggs. Among other soil characteristics, TOC and clay content were related with lower and higher egg concentrations for most PFAAs, respectively. This suggests that bioavailability of PFAAs to the eggs is driven by complex physicochemical interactions of PFAAs with TOC and clay. Finally, remediation measures were formulated that are readily applicable to lower PFAA exposure via homegrown eggs.