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Issue 8, 2002
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Determination of 236U/238U isotope ratio in contaminated environmental samples using different ICP-MS instruments

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Abstract

This paper considers use of the 236U isotope to monitor the spent uranium from nuclear fallout using inductively coupled plasma mass spectrometry (ICP-MS) in soil samples collected in the vicinity of the Chernobyl Nuclear Power Plant (NPP). Sector field ICP-MS (ICP-SFMS) and quadrupole based ICP-MS without and with hexapole collision cell (ICP-CC-MS) were used for uranium isotope analysis. In addition, a multiple ion collector ICP-MS (MC-ICP-MS) was used for high-precision isotope ratio measurements. A 238U+ ion sensitivity of 18 GHz ppm−1, 12.4 GHz ppm−1 and 16 GHz ppm−1, respectively, was observed in ICP-SFMS, ICP-CC-MS and MC-ICP-MS with ultrasonic nebulizer. An absolute sensitivity of 3600 counts fg−1 was achieved for uranium by using a direct injection high efficiency nebulizer for solution introduction in ICP-SFMS. The detection limit for 236U was in the fg g−1 range and abundance ratio sensitivity for 236U/238U was 5 × 10−6, 3 × 10−7, 6 × 10−7, and less than 3 × 10−7 in ICP-SFMS, MC-ICP-MS, quadrupole ICP-MS and ICP-CC-MS at mass resolution mm = 300, respectively. Interlaboratory comparison yielded a good accuracy (0.4–1.6%) of 236U/238U isotope ratios ranging from 1.5 × 10−3 to 3.2 × 10−4 measured in samples containing 100 ng of uranium. The 236U/238U isotope ratios and spent uranium fraction were determined in Chernobyl soil samples using single ion detector ICP-MS and multiple ion collector ICP-MS (MC-ICP-MS). In comparison to 235U/238U isotope ratio, the 236U/238U isotope ratio provided more sensitive and accurate determination of the portion of spent uranium from Chernobyl NPP in spent/natural uranium mixture in soil samples down to 0.1%. The concentration of Chernobyl spent uranium in upper 0–10 cm soil layers in investigated areas in the vicinity of Chernobyl NPP amounts to 2.4 × 10−9 g g−1 to 8.1 × 10−7 g g−1 depending mainly on the distance to the Chernobyl reactor.

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Article information


Submitted
19 Feb 2002
Accepted
05 Jun 2002
First published
27 Jun 2002

J. Anal. At. Spectrom., 2002,17, 958-964
Article type
Paper

Determination of 236U/238U isotope ratio in contaminated environmental samples using different ICP-MS instruments

S. F. Boulyga, J. L. Matusevich, V. P. Mironov, V. P. Kudrjashov, L. Halicz, I. Segal, J. A. McLean, A. Montaser and J. Sabine Becker, J. Anal. At. Spectrom., 2002, 17, 958
DOI: 10.1039/B201803A

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