Determination of Depleted Uranium in Urine via Isotope Ratio Measurements Using Large-Bore Direct Injection High Efficiency Nebulizer-Inductively Coupled Plasma Mass Spectrometry

摘要

Inductively coupled plasma mass spectrometry (ICP-MS), coupled with a large-bore direct injection high efficiency nebulizer (LB-DIHEN), was utilized to determine the concentration and isotopic ratio of uranium in 11 samples of synthetic urine spiked with varying concentrations and ratios of uranium isotopes. Total U concentrations and ~(235)U/~(238)U isotopic ratios ranged from 0.1 to 10 μg/L and 0.0011 and 0.00725, respectively. The results are compared with data from other laboratories that used either α-spectrometry or quadrupole-based ICP-MS with a conventional nebulizer-spray chamber arrangement. Severe matrix effects due to the high total dissolved solid content of the samples resulted in a 60 to 80% loss of signal intensity, but were compensated for by using ~(233)U as an internal standard. Accurate results were obtained with LB-DIHEN-ICP-MS, allowing for the positive identification of depleted uranium based on the ~(235)U/~(238)U ratio. Precision for the ~(235)U/~(238)U ratio is typically better than 5% and 15% for ICP-MS and α-spectrometry, respectively, determined over the concentrations and ratios investigated in this study, with the LB-DIHEN-ICP-MS system providing the most accurate results. Short-term precision (6 min) for the individual ~(235)U and ~(238)U isotopes in synthetic urine is better than 2% (N=7), compared to ～5% for conventional nebulizer-spray chamber arrangements and >10% for α-spectrometry. The significance of these measurements is discussed for uranium exposure assessment of Persian Gulf War veterans affected by depleted uranium ammunitions.