Abstract
We present a new analytical method for accurately measuring femtogram amounts of Pu in environmental swipe samples using a high-purity 244Pu spike and multi-collector inductively-coupled-plasma mass spectrometry. The method was validated by comparative measurements of samples that were previously analysed using a 242Pu spike. The 244Pu spike allows direct normalization of all Pu isotopes to both 244Pu and 239Pu, along with online monitoring of PbAr interferences, resulting in highly-sensitive and accurate Pu assay and isotope ratio measurements. Expanded uncertainties were typically < 2.5% for Pu amounts larger than 20 fg, and < 1% for Pu isotope ratios larger than 0.08. Detection thresholds (Lc) were well below 1 fg for all Pu isotopes.
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Notes
The “242Pu method” has been in use at the IAEA ESL since 2013, and differs from the method described by Eppich et al. [18] in 2019. The published method [18] represented an experimental study for the determination of Pu assay and isotope ratios in swipe samples when using a 242Pu spike. However, that method has not been fully implemented for routine Pu analysis.
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Acknowledgements
We thank Herbert Siegmund, Guillaume Stadelmann and Gary R. Eppich for their support in equipment troubleshooting and for the valuable discussions on the subject of this paper. Zsuzsanna Mácsik is acknowledged for her help in the selection of archived swipe samples for comparison measurements, and for the initial preparation and amount verification of the used 244Pu CRM at the IAEA ESL. Beata Varga is acknowledged for her advice during the validation of this method. Alena Bulyha and Alexander Venzin are acknowledged for developing Visual Basic and R-codes for uncertainty calculations and data evaluation automation. Furthermore, the authors would like to thank Renáta Buják for her review and for providing insightful comments.
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Konegger-Kappel, S., Koepf, A., Katona, R. et al. A new era of plutonium assay and isotope ratio measurements at ultra-low levels in IAEA safeguards environmental swipe samples by isotope dilution MC-ICP-MS using a 244Pu spike. J Radioanal Nucl Chem 332, 2887–2904 (2023). https://doi.org/10.1007/s10967-023-08880-x
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DOI: https://doi.org/10.1007/s10967-023-08880-x