Sedimentary records of metal deposition in Japanese alpine lakes for the last 250 years: Recent enrichment of airborne Sb and In in East Asia

Concentrations of 18 elements, including Sb, In, Sn, and Bi, were measured in sediment cores from two pristine alpine lakes on Mount Hachimantai, northern Japan, representing the past 250 years. Vertical variations in concentrations are better explained by atmospheric metal deposition than by diagenetic redistribution of Fe and Mn hydroxide and organic matter. Anthropogenic metal fluxes were estimated from 210Pb-derived accumulation rates and metal concentrations in excess of the Al-normalized mean background concentration before 1850. Anthropogenic fluxes of Sb and In showed gradual increases starting around 1900 in both lakes, and marked increases after 1980. Comparison of Sb/Pb and Pb stable isotope ratios in sediments with those in aerosols of China or northern Japan and Japanese source materials (recent traffic- and incinerator-derived dust) suggest that the markedly elevated Sb flux after 1980 resulted primarily from enhanced long-range transport in aerosols containing Sb and Pb from coal combustion on the Asian continent. The fluxes of In, Sn, and Bi which are present in Chinese coal showed increasing trends similar to Sb for both study lakes. This suggests that the same source although incinerators in Japan may not be ruled out as sources of In. The sedimentary records for the last 250 years indicate that atmospheric pollution of Sb and In in East Asia have intensified during recent decades. -- Highlights: ► First report on historical trends in Sb and In enrichment in East Asian atmosphere ► Sedimentary records show a marked increase of Sb and In depositions since 1980. ► Sb/Pb ratios suggest coal combustion in East Asia as an important source of Sb. ► Atmospheric pollution of Sb and In intensified in East Asia during recent decades