Siskiwit Lake revisited:: Time trends of polychlorinated dibenzo-p-dioxin and dibenzofuran deposition at Isle Royale, Michigan

We have investigated the time trends of polychlorinated dibenzo-p-dioxins and polychlorinated dibenzofurans (PCDD/F) in two dated sediment cores from Siskiwit Lake, a remote lake on Isle Royale in Lake Superior. Both cores indicated that atmospheric deposition of PCDD/F to Siskiwit Lake increased sharply in the 1930s and peaked in the late 1970s at around 9.5 pg cm(-2)yr(-1). Since then, atmospheric deposition to Siskiwit Lake has continued to decline. Analysis of the top 1.0 cm of these cores showed that in 1996-1998, the PCDD/F flux to Siskiwit Lake was about 4.5 pg cm(-2) yr(-1). We compared this sediment-derived flux to a soil-derived flux from Ryan Island, the largest island in Siskiwit Lake, and found a similar value. Thus, the atmospheric deposition of PCDD/F has decreased about 50% since the late 1970s. This decline is slower than might be expected as a result of combustion source regulations alone. Examination of the PCDD/F homologue distributions throughout the sediment cores showed that the relative percent of the hepta- and octachlorinated dibenzo-p-dioxins to total PCDD/F increased with time. We propose that de novo synthesis of these compounds from pentachlorophenol in the atmosphere explains these data.