Legacy and novel brominated flame retardants in agricultural soils of eastern China (2011-2021): Concentration level, temporal trend, and health risk assessment.

Polybrominated diphenyl ethers (PBDEs) and novel brominated flame retardants (NBFRs) have been extensively investigated in the terrestrial environment of China. However, little is known about how PBDEs and NBFRs burdens in agricultural soils altered over time. In this study, agricultural soils from different regions of China were collected from 2011 to 2021 to investigate the contamination levels and temporal variation of PBDEs and NBFRs. The concentrations of ∑PBDEs and ∑NBFRs ranged from 0.144 to 215 ng/g dry weight (d.w.) and 0.186-144 ng/g (d.w.), with a mean value of 9.27 ng/g (d.w.) and 8.22 ng/g (d.w.), respectively. Among PBDEs and NBFRs, BDE-209 and decabromodiphenylethane (DBDPE) were the most predominant compounds. The PBDE concentrations did not vary significantly during the past decade, whereas the lower brominated congeners increased with time (doubling times ranged from 5.46 to 8.56 years). Meanwhile, NBFR concentrations increased over time, with concentrations significantly higher in 2021, 2016, and 2013 than in 2011 (p < 0.05). Additionally, DBDPE, 1,2-bis(2,4,6-tribromophenoxy)ethane (BTBPE), and hexabromobenzene (HBB) had doubling times of 6.84, 11.2, and 7.37 years, respectively. Total organic matter (TOC) impacted the distribution and variation of PBDEs (particularly lower-brominated congeners), with soil organic matter (SOM)-sorption showing an increasing and then decreasing trend. Health risk assessment suggested that PBDEs and NBFRs did not pose non-carcinogenic risks to humans. Nevertheless, the long-term health risk of BFRs should be considered. Overall, this is the first study to comprehensively analyze the contamination burdens and temporal trends of PBDEs and NBFRs in Chinese agricultural soils over a long period, providing a fundamental basis for future BFR management.