Precise age determination of a single plutonium particle using inductively coupled plasma mass spectrometer

Abstract

Age-dating of single plutonium oxide particles ∼ 1 μm in diameter was demonstrated using eight particles. For this demonstration, the particles were prepared from a standard reference material SRM-947 that had been stored for 3.9 years since the last Pu purification. The Pu particles were separately dissolved, and Am and Pu were chemically separated from the solution via anion-exchange chromatography. The isotope ratios of Am and Pu in the eluted fractions were measured using a high-resolution inductively coupled plasma mass spectrometer (HR-ICP-MS). The precision and accuracy of the Pu age were improved through the addition of an 243 Am spike to the sample solutions and by the trace chemical separation of Pu and Am. The determined age in this work was in good agreement with the expected age with high accuracy (deviation: 7.1-105 days) and precision (uncertainty: 0.16-0.5 years (k = 1)). These results indicate that a combination of ICP-MS and chemical separation after spiking with 243 Am provides an effective tool for the analysis of environmental samples collected during nuclear safeguard inspections.

Mass spectrometric analysis for nuclear safeguards

“…126 Recently, procedures for age-dating of single Pu particles by using SIMS, TIMS and ICP-MS have been reported. [130][131][132] Miyamoto et al 132 implemented chemical separation of Pu and Am in individual particles aer spiking them with 243 Am. The obtained results indicate the suitability of the developed technique for dating of Pu particles from environmental samples collected during nuclear safeguards inspections.…”

Atomic spectrometry update: review of advances in atomic spectrometry and related techniques

“…Ezerinskis et al 128 described a method to evaluate the abundance of 129 I using ion chromatography combined with ICP-SFMS. Individual 1 mm plutonium particles have been analysed via HR-ICP-MS by Miyamoto et al 130 with the objective of measuring the time since last Pu purication. Uranium isotope measurement of micrometre-scale particles was the subject of a study by Hubert et al 129 A femtosecond laser-ICP-MS combination optimised for laser shot repetition rate produced reproducibility of 238 U: 235 U better than 4% from <200 pg U.…”

Atomic spectrometry update: review of advances in atomic spectrometry and related techniques

“…Uranium isotope measurement of micrometre-scale particles was the subject of a study by Hubert et al 129 A femtosecond laser-ICP-MS combination optimised for laser shot repetition rate produced reproducibility of 238 U: 235 U better than 4% from <200 pg U. Individual 1 mm plutonium particles have been analysed via HR-ICP-MS by Miyamoto et al 130 with the objective of measuring the time since last Pu purication. HR-ICP-MS and a 243 Am spike were used to determine the age, which could be constrained between uncertainties of 2 and 6 months.…”

“…These authors did not identify any Ba isotope fractionation on column recovery of 89% within the bounds of the measurement uncertainty (d 137:134 Ba AE 0.025&). Mass dependent fractionation during MC-ICP-MS analysis was corrected using a [130][131][132][133][134][135] Ba double spike and massindependent fractionation was accounted for by standardsample bracketing. The d 137:134 Ba precision documented in this study is a factor of ve better than achieved previously and was sufficient to identify differences between three igneous rock reference standards (JB-2, JA-2 and BHVO-2).…”