Determination of U-236 and transuranium elements in depleted uranium ammunition by alpha spectrometry and ICP-MS

It is well known that ammunition containing depleted uranium (DU) was used by NATO during the Balkan conflict. To evaluate the origin of DU (the enrichment of natural uranium or the reprocessing of spent nuclear fuel) it is necessary to directly detect the presence of activation products (236U, 239Pu, 240Pu, 241Am, and 237Np) in the ammunition. In this work the analysis of actinides by α-spectrometry was compared with that by inductively coupled plasma mass spectrometry (ICP-MS) after selective separation of ultratraces of transuranium elements from the uranium matrix. 242Pu and 243Am were added to calculate the chemical yield. Plutonium was separated from uranium by extraction chromatography, using tri-n-octylamine (TNOA), with a decontamination factor higher than 106; after elution plutonium was determined by ICP-MS (239Pu and 240Pu) and α-spectrometry (239+240Pu) after electroplating. The concentration of Pu in two DU penetrator samples was 7×10-12g g-1 and 2×10-11g g-1. The 240Pu/239Pu isotope ratio in one penetrator sample (0.12±0.04) was significantly lower than the 240Pu/239Pu ratios found in two soil samples from Kosovo (0.35±0.10 and 0.27±0.07). 241Am was separated by extraction chromatography, using di(2-ethylhexyl)phosphoric acid (HDEHP), with a decontamination factor as high as 107. The concentration of 241Am in the penetrator samples was 2.7×10-14g g-1 and <9.4×10-15g g-1. In addition 237Np was detected at ultratrace levels. In general, ICP-MS and α-spectrometry results were in good agreement. The presence of anthropogenic radionuclides (236U, 239Pu, 240Pu, 241Am, and 237Np) in the penetrators indicates that at least part of the uranium originated from the reprocessing of nuclear fuel. Because the concentrations of radionuclides are very low, their radiotoxicological effect is negligible.