Spatiotemporal transitions of organophosphate esters (OPEs) and brominated flame retardants (BFRs) in sediments from the Pearl River Delta, China

Recent regulations on the use of brominated flame retardants (BFRs, especially polybrominated diphenyl ethers, PBDEs) have led a sharp increase in the use of organophosphate esters (OPEs), which have become the subject of widespread environmental concern. To gain insights into their environmental transitions, we investigated the spatiotemporal trends and sources of 25 OPEs and 23 BFRs (21 PBDEs and two alternative BFRs) in sediments from the Pearl River Delta (PRD), the second economic/industrial region of China. Among them, PBDEs showed higher mean concentrations than OPEs and alt-BFRs in PRD sediments, a continual increase in most PRD areas, and positive correlations with most local socioeconomic parameters. The source analysis results indicated that all of these changes resulted from the substantial use/stock of PBDEs (especially deca-BDE) in this region, and BDE-209 displayed debromination in most sediments. OPEs demonstrated obvious increases in sediments from all major PRD rivers, especially those located in less-developed regions. This distribution might be related to the large-scale industry relocation from the central PRD area to its vicinities. Unexpectedly, decabromodiphenyl ethane (DBDPE), an important deca-BDE substitute, presented considerable declines in the PRD sediments while several novel OPEs showed considerably high proportions, especially aryl-substituted OPEs, which merit further screening analysis. [Display omitted] •OPEs, PBDEs and alt-BFRs in PRD sediments held distinct spatiotemporal trends.•OPEs in PRD sediments rose visibly following the ban of PBDEs while alt-BFRs fell.•PBDEs kept rising in most PRD sediments due to their substantial historical use.•Unlike BFRs, OPEs showed insignificant correlation with local socioeconomic values.•Novel OPEs showed considerable proportions and merit further screening analysis.