Spatially-resolved uranium isotopic analysis of contaminated scrap metal using laser ablation multi-collector ICP-MS.

Laser ablation multi-collector inductively coupled plasma mass spectrometry (LA-MC-ICP-MS) was applied to the detailed investigation of the uranium (U) isotopic composition (U, U, U, and U) of five contaminated scrap metal samples found within the European Union. Pressed pellets of the two certified U isotopic reference materials CRM U-020 and CRM U-030 were included in the measurement protocol for mass bias correction, calculation of the ion counter gains and for quality assurance. Since the investigated samples had low U content (0.15-14.3 wt%) compared to typically analysed pure U compounds (>60 wt%), the applied experimental parameters had to be adjusted. Spatially-resolved U isotopic information was obtained by line scan analysis of each sample. While other analytical techniques used typically in nuclear forensic investigations, such as γ-spectrometry and thermal ionisation mass spectrometry (TIMS) yielded average U isotopic compositions of the entire sample, LA-MC-ICP-MS provided substantial added value, highlighting the inhomogeneous distribution of U isotopes within various scrap metal samples. Analysis of individual particles secondary ion mass spectrometry (SIMS) confirmed the large range of U enrichment levels in heterogeneous scrap metal samples. Four out of five scrap metal samples contained U (∼0.05-∼0.11 wt%), indicating the presence of reprocessed U. Taken together, LA-MC-ICP-MS analysis provided fast and accurate spatially-resolved U isotopic information without consuming or altering the scrap metal samples, a key feature for nuclear forensics investigations.