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Direct, uncorrected, molecule-free analysis of 236U from uranium-bearing particles with NAUTILUS: a new kind of mass spectrometer

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Abstract

We demonstrate use of the Naval Ultra-Trace Isotope Laboratory's Universal Spectrometer (NAUTILUS) at the U.S. Naval Research Laboratory (NRL) to measure 236U directly from uranium-bearing particles free from molecular isobaric interferences. Particles with 235U enrichments in the range of 0.32% to 3.28% and 236U enrichments from no enrichment to 0.015% provided by the International Atomic Energy Agency (IAEA) were analyzed directly using the NAUTILUS. We report the experimental data here without correcting for molecular hydrides and/or applying any other background subtractions. The results from all samples agreed with the certified values within standard error save for the 236U composition of the IRMM 023, which suffered from a combination of insufficient particle sizes and sub-μmol mol−1 236U concentrations. We were able, however, to directly measure as low as three μmol mol−1 of 236U in individual particles regardless of the 235U concentration. Our results are comparable with Large Geometry Secondary Ion Mass Spectrometry (LG-SIMS) and serve as baseline for a more comprehensive comparison between LG-SIMS and the NAUTILUS in the future. Moreover, we demonstrate the ability of the NAUTILUS to generate raster ion images with the same ease as traditional LG-SIMS instruments. By combining our ability to measure 236U directly with raster ion imaging, we were able to detect a low intensity, small uranium-bearing particle in the presence of high molecular backgrounds for a non-ideal sample. This discovery could lead to more targeted and, therefore, less time intensive particle screening methodologies.

Graphical abstract: Direct, uncorrected, molecule-free analysis of 236U from uranium-bearing particles with NAUTILUS: a new kind of mass spectrometer

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Publication details

The article was received on 30 Jul 2018, accepted on 06 Sep 2018 and first published on 07 Sep 2018


Article type: Paper
DOI: 10.1039/C8AN01451E
Citation: Analyst, 2018, Advance Article
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    Direct, uncorrected, molecule-free analysis of 236U from uranium-bearing particles with NAUTILUS: a new kind of mass spectrometer

    D. Willingham, E. E. Groopman, K. S. Grabowski and L. Sangely, Analyst, 2018, Advance Article , DOI: 10.1039/C8AN01451E

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