Determination of plutonium isotopes in freshwater lake sediments by sector-field ICP-MS after separation using ion-exchange chromatography

The determination of Pu isotopes in lake sediments is important for many studies, such as Pu pollution source identification, sediment mixing estimation, erosion evaluation and establishment of deposition chronology in lakes. In this paper, a simple analytical method using sector field inductively coupled plasma mass spectrometry (ICP-MS) combined with two-stage chromatographic separation and purification of Pu was developed based on the optimization and adaptation of the previously published method for marine samples with an emphasis on the study of the elimination of interferences for the analysis of freshwater lake sediments. A strong base anion-exchange resin (AG MP-1M) was used to purify Pu isotopes with concentrated HBr as the final eluent for Pu elution. The chemical yields were ca. 64% and the decontamination factor for U was ca. 10(5). The developed method was validated using a freshwater lake sediment reference material (SRM-4354) and a marine sediment reference material (IAEA-368), and applied to the determination of Pu isotopes in sediment samples of Lake Poyang, East China. For the analysis of certified reference materials, both Pu239+240 activity of 31.6mBqg(-1), and Pu-240/Pu-239 atom ratio of 0.033 for IAEA-368 were comparable to the certified value and/or literature values. As for SRM-4354, Pu239+240 activity of 3.90 mBqg(-1) agreed well with the certified value. However, the mean Pu-240/Pu-239 atom ratio of 0.144 was lower than those reported by other laboratories. This difference suggested that this material may be isotopically inhomogeneous. Pu-240/Pu-239 atom ratios of Poyang Lake sediment samples ranged from 0.185 to 0.192 with a mean value of 0.187 +/- 0.004, indicating that plutonium pollution originated from global fallout. (c) 2008 Elsevier Ltd. All rights reserved.