Direct uranium isotope ratio analysis of single micrometer-sized glass particles

• Published in: Journal of environmental radioactivity 2012-11, Vol.113 (8), p.8-15
• Main Authors: Kappel, Stefanie, Boulyga, Sergei F., Prohaska, Thomas
• Format: Article
• Language: English
• Subjects: Applied sciences; Energy; Energy. Thermal use of fuels; Exact sciences and technology; Fission nuclear power plants; Glass - analysis; Installations for energy generation and conversion: thermal and electrical energy; Isotopes - analysis; Laser ablation; Mass Spectrometry; Multi collector ICP-MS; Nuclear forensics; Nuclear safeguards; Particle analysis; Particle Size; Uranium - analysis; Uranium isotope ratio analysis
• ISSN: 0265-931X; 1879-1700
• DOI: 10.1016/j.jenvrad.2012.03.017

We present the application of nanosecond laser ablation (LA) coupled to a ‘Nu Plasma HR’ multi collector inductively coupled plasma mass spectrometer (MC-ICP-MS) for the direct analysis of U isotope ratios in single, 10–20 μm-sized, U-doped glass particles. Method development included studies with respect to (1) external correction of the measured U isotope ratios in glass particles, (2) the applied laser ablation carrier gas (i.e. Ar versus He) and (3) the accurate determination of lower abundant 236U/238U isotope ratios (i.e. 10−5). In addition, a data processing procedure was developed for evaluation of transient signals, which is of potential use for routine application of the developed method. We demonstrate that the developed method is reliable and well suited for determining U isotope ratios of individual particles. Analyses of twenty-eight S1 glass particles, measured under optimized conditions, yielded average biases of less than 0.6% from the certified values for 234U/238U and 235U/238U ratios. Experimental results obtained for 236U/238U isotope ratios deviated by less than −2.5% from the certified values. Expanded relative total combined standard uncertainties Uc (k = 2) of 2.6%, 1.4% and 5.8% were calculated for 234U/238U, 235U/238U and 236U/238U, respectively. ► LA-MC-ICP-MS was fully validated for the direct analysis of individual particles. ► Traceability was established by using an IRMM glass particle reference material. ► Measured U isotope ratios were in agreement with the certified range. ► A comprehensive total combined uncertainty evaluation was performed. ► The analysis of 236U/238U isotope ratios was improved by using a deceleration filter.