Sources of the transuranic elements plutonium and neptunium in arctic marine sediments

We report here thermal ionization mass spectrometry measurements of 239Pu, 240Pu, 241Pu, 242Pu, and 237Np isolated from oceanic, estuarine, and riverine sediments from the Arctic Ocean Basin. 238Pu/239+240Pu activity ratios are also reported for alpha spectrometric analyses undertaken on a subset of these samples. Our results indicate that the Pu in sediments on the Alaskan shelf and slope, as well as that in the deep basins (Amerasian and Eurasian) of the Arctic Ocean, has its origin in stratospheric and tropospheric fallout. Sediments from the Ob and Yenisei Rivers show isotopic Pu signatures that are distinctly different from those of northern-hemisphere stratospheric fallout and indicate the presence of weapons-grade Pu originating from nuclear fuel reprocessing wastes generated at Russian facilities within these river catchments. Consequently, sediments of the Eurasian Arctic Ocean, particularly those in the Barents and Kara Seas, probably contain a mixture of Pu from stratospheric fallout, tropospheric fallout, and fuel-reprocessing wastes of riverine origin. In particular, the 241Pu/239Pu ratios observed in these sediments are inconsistent with significant contributions of Pu to the arctic sediments studied from western European reprocessing facilities, principally Sellafield in the UK. Several other potential sources of Pu to arctic sediments can also be excluded as significant based upon the transuranic isotope ratios presented.