Are unintentionally produced polychlorinated biphenyls the main source of polychlorinated biphenyl occurrence in soils?

Highlights: • Ln PCB concentrations linearly decrease with distances from the city. • PCB emission inventory in the Bohai and Yellow Sea Rim was estimated. • Quantitative source identification was conducted using fugacity model method. • Low-chlorine PCBs in soils mainly came from recent 5-year emissions. • Unintentionally produced PCB emissions are the major contributors to PCBs in soils. The production of polychlorinated biphenyls (PCBs) has been banned globally for decades, but PCB concentrations in environmental media remain relatively high, especially in urban areas. Emissions estimates, studies of soil gradients between urban and rural areas, and quantitative identification of regional sources of PCBs in soils are necessary for understanding the environmental behavior of PCBs. In this study, regional PCB emissions were estimated at a resolution of 10 km × 10 km, and the spatial distribution of soil PCBs from urban to rural areas was studied along the Bohai and Yellow Sea regions. Compared with rural areas, mean PCB concentrations in urban soils (20.7 ng/g) were found to be higher, and concentrations decreased with distance from the city. Across both latitude and longitude directions, high PCB emissions in urban areas matched the distribution of total PCB concentrations in soils. The concentrations of the pollutants PCB28, PCB52, PCB101, PCB118, PCB138, PCB153, and PCB180 in soils originated from 5-year emissions, and accounted for 97%, 95%, 84%, 81%, 58%, 57%, and 27% of the total emissions, respectively. Unintentionally produced PCB (UP-PCB) emissions, which are mainly derived from cement (42%), pig iron (37%), crude steel (18%), and rolled steel (3%) industries, are the major contributors to PCBs in soils. Further identification of the sources and fates of PCBs requires a combination of field, laboratory, and modeling efforts.