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Isotopic composition of commercially available uranium chemicals and elemental analysis standards

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Abstract

Reference information on isotopic composition of various uranium materials, determined with high accuracy and precision, is of essential value for nuclear safeguards and nuclear forensics. In addition, an accurate knowledge of the isotopic composition is important when isotope-specific measurement techniques such as inductively-coupled plasma mass spectrometry (ICP-MS) are employed for elemental analysis. Isotopic composition of ten uranium chemicals and standards for elemental analysis, acquired from various commercial suppliers, was measured using thermal ionisation mass spectrometry in the modified total evaporation mode. Two of the chemicals analyzed are based on either natural uranium (NU) or ‘commercial NU’. The majority of the materials were found to contain uranium substantially depleted in 234U and 235U, with presence of 236U significantly above the range observed for NU. Model scenarios are suggested for a combination of uranium irradiation and enrichment processes which may have resulted in such compositions.

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Notes

  1. WIMS stands for Winfrith improved multigroup reactor [code] scheme. Winfrith Atomic Energy Establishment was a UK Atomic Energy Authority site near Winfrith Newburgh in Dorset. FISPIN is an acronym of FISsion Products INventory.

  2. The N reactor only began operation in 1963. However, our simplistic assumption is that although design of reactors at the Hanford site evolved over time [38], they all were of the same generic type (NU-fuelled, graphite moderated, light water cooled), and hence, for the Hanford reactors, differences in change of uranium isotopic composition with the fuel burnup are negligible.

  3. For comparison: Bukharin [2] stated that Soviet military programme generated RU with 0.667% 235U; this corresponds to irradiation of NU fuel to about 550 MWd/tU and generation of plutonium with approximately 96% 239Pu.

  4. Notable is the inconsistency of available information about enrichment level of the Paducah product. While Smith [39] provides detailed data ranging from 0.89 to 1.95% 235U, Diehl [37] claims an average of 2.75% 235U. We used the both data sources for the enrichment cascade modelling, however only the models based on data from [39] are presented in this paper.

  5. Notable is an apparent internal inconsistency in the data presented on this subject in [37]: while for the 1965–1968 time period (as well as for 1982) “% of reactor tails in total feed” is shown at zero level, the 236U in the enrichment tails remained within the 0.002–0.003% range; the latter assumes a significant proportion of RU in the feed. For 1969–1970 the RU fraction is shown at 25–35%; the latter figure is close to our estimation.

  6. When making such assumptions one should keep in mind that neither the Hanford reactors nor the Paducah gaseous diffusion cascades were unique in their generic design, characteristics and use during the Cold War era. For example, according to Bukharin [2], USSR enriched RU from 0.67% to 90% 235U using gaseous diffusion (1950–1962) or gas centrifuge (1962–1988) cascades, generating average tails with 0.36% and 0.30% 235U, respectively. It is not clear whether the RU feed was mixed with NU, and if there were intermediate enrichment steps. In general, while the production sites and scenarios considered in the current work may have generated uranium isotopic compositions consistent with several of the analyzed samples, some other combinations of irradiation, recycling and enrichment processes cannot be ruled out as possible sources for the DU found in these materials.

  7. One possible scenario involves re-enrichment of near-natural feed (0.72% 235U) consisting of RU from the weapon-grade Pu production in a NU-fuelled heavy water moderated reactor and a tiny proportion (less than 0.2%) of unirradiated HEU. However, although theoretically plausible, this scenario does not appear realistic.

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Acknowledgments

The authors are grateful to Ahmed El Gebaly for his efforts to identify potential suppliers of uranium chemicals, and to Tobias Petersmann who arranged for procurement of the selected materials. The MSTAR software was provided to the IAEA Department of Safeguards under the US Support Programme Task A 1498. The WIMS-FISPIN calculations were carried out under the UK Support Programme Task A 1853. Greatly appreciated are the valuable comments to this paper manuscript made by three anonymous reviewers.

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Authors and Affiliations

  1. Department of Safeguards, International Atomic Energy Agency, Vienna International Centre, PO box 100, 1400, Vienna, Austria

    M. Peńkin, S. Boulyga, B. Dabbs, D. Fischer, M. Humphrey, A. Kochetkov, A. Koepf & M. Sturm

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  1. M. Peńkin
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Correspondence to M. Peńkin.

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Peńkin, M., Boulyga, S., Dabbs, B. et al. Isotopic composition of commercially available uranium chemicals and elemental analysis standards. J Radioanal Nucl Chem 316, 791–798 (2018). https://doi.org/10.1007/s10967-018-5740-5

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