Historical trends of traditional, emerging, and halogenated polycyclic aromatic hydrocarbons recorded in core sediments from the coastal areas of the Yellow and Bohai seas

Abstract

Historical trends of polycyclic aromatic hydrocarbons (PAHs) contamination were reconstructed from eleven sediment cores located in intertidal zones of the Yellow and Bohai seas for a period encompassing the last 80 years. The analysis encompassed 15 traditional PAHs (t-PAHs), 9 emerging PAHs (e-PAHs), and 30 halogenated PAHs (Hl-PAHs), including 10 chlorinated PAHs (Cl-PAHs) and 20 brominated PAHs (Br-PAHs). Concentrations of target PAHs were highest in industrial and municipal areas situated along the coast of the Bohai Sea, including Huludao, Yingkou, Tianjin, and Dandong, constituting a substantial mass inventory. All target PAHs showed increasing trends since the 1950s, reflecting the development history of South Korea and China. High molecular weight PAHs accumulated in sampling sites more than low molecular weight PAHs. A positive matrix factorization model showed that the PAH sources were coal and gasoline combustion (35%), diesel combustion (33%), and biomass combustion (32%). Over the last 80 years, the contribution of coal and gasoline combustion increased in all regions, while diesel combustion and biomass combustion varied across regions and over time. Toxicity equivalence values were highest for t-PAHs (>99% contribution), followed by Cl-PAHs, Br-PAHs, and e-PAHs. Concentrations of t-PAHs in Eastern Asia seas have increased since the 1900s, particularly in intertidal areas compared to subtidal areas. The intertidal zone removed 83% of the total flux of PAHs originating from land and thus appears to serve as a buffer zone against marine pollution. Overall, this study provides novel knowledge on the historical trends and sources of PAHs on a large scale, along with insights for future coastal management.