Sources and Fates of Sedimentary Polycyclic Aromatic Hydrocarbons in the East Siberian Arctic Shelf: Implications for Input Pathways and Black Carbon Constraint

Abstract

The Arctic region is experiencing more rapid climate changes than the other parts of the world and serves as a sink for semi-volatile persistent organic pollutants, such as polycyclic aromatic hydrocarbons (PAHs), which can be utilized as molecular markers for pyrogenic carbon, such as black carbon (BC). As the sea ice retreats and increased terrestrial inputs with widespread wildfires, the PAH concentrations in the Arctic Ocean are rising. In this study, the sources and fates of PAHs together with BC in surface sediments from the East Siberian Arctic Shelf (ESAS) were analyzed. Positive matrix factorization (PMF) elucidated a mixed petrogenic and pyrogenic sources and distinct PAH fates associated with diverse input pathways including coastal permafrost erosion contribution (∼30%), petrogenic-related emission (∼34%), fossil fuel combustion (∼26%), and biomass burning (∼10%). Correlation analysis indicated that BC plays a key role in affecting the behavior and fates of PAHs. In the Chukchi Sea, PAHs are closely associated with soot-BC, whereas in the Laptev Sea (LS) and west East Siberian Sea (W-ESS), they exhibit a coupling process with char-BC. The presence of these carbonaceous materials in the sediments of CS is likely influenced by atmospheric deposition and biological activity, whereas the LS and W-ESS regions are mainly affected by long-distance river transport and direct deposition from coastal permafrost. As global warming continues, permafrost thawing induces the remobilization and retranslocation of PAHs, thereby becoming a significant PAH contributor and input pathway in the rapidly changing Arctic coastal margin.