The spatial-temporal evolution of heavy metal accumulation in the offshore sediments along the Shandong Peninsula over the last 100 years: Anthropogenic and natural impacts

The anthropogenic and natural impacts on the temporal and spatial variations of heavy metals in sediments under the Shandong Peninsula coastal current are still unclear. Here, the concentrations\burial fluxes of Cr, Cu, Zn, As, and Pb in three sediment cores retrieved from the Bohai Sea and the Yellow Sea along the Shandong Peninsula were analyzed to study the spatial-temporal variability of heavy metal accumulation over the last century. The results showed that the buried heavy metal fluxes were relatively low at the end of the Shandong Peninsula coastal current. The enrichment factor (EF) and geoaccumulation index (I-geo) indicated that those metals did not severely pollute the sediments except As that reached a moderate enrichment. Principal component analysis (PCA) revealed that Cr, Cu, Zn, and Pb were mainly derived from natural weathering and As was determined by anthropogenic contamination. The strength of the Shandong Peninsula coastal current, the Yellow River estuary location, and sediment discharge load significantly influenced the concentrations of natural-origin heavy metals by affecting sediment grain size and the source-sink process. The emission of pollutants from agricultural and industrial activities in the Shandong Peninsula region resulted in As enrichment since the 1950s. Moreover, the EF values of heavy metals in sediment cores from China's coastal seas showed apparent spatial variations of heavy metal pollution but had coherent temporal variability with China's economic development process. Heavy metals pollution has weakened in most coastal seas since the 2000s, likely due to the extensive industrial upgrading and the implementation of pollution control. These results have a reference significance for studying the evolution and source-sink process of the heavy metals in offshore sediments and tracing anthropogenic impacts in different periods.