Intentional Uranium Tagging for Material Provenance and Pathway Forensics (LA19-Intentional-Forensics-NDD3Bb) (Annual Report for FY21)
This report describes the outcomes of the third and final year of a project to research the feasibility of tagging uranium materials, especially nuclear fuels. The experimental focus remained on metallic uranium forms under prospective surface and bulk tagging scenarios. Overall, the results showed that the tags could be successfully imparted and characterized in both as-built and degraded conditions. This was in line with expectations coming into this project, indicating promise for both surface and bulk tagging of metallic forms of uranium. Multiple surface tagging techniques and detection strategies were explored in FY21, with an emphasis on improving tag quality, readability, and detection in the field. Non-radioactive materials were used as a testbed. Selective deposition via laser beam was determined to be successful in imparting a readable titanium deposit on a stainless steel base plate, and can be read with high resolution characterization techniques (e.g., scanning electron microscopy) and field capable tools (e.g., eddy current testing). Other deposition techniques, such as selective deposition via electron beam and photoluminescent tags, were explored in FY21, and while success for these techniques would be dependent on additional work, these techniques showed potential for surface tagging applications. To survey bulk taggant elements for bulk uranium metal, 16 tagging elements were spread among 18 depleted uranium castings (4 baseline, 3 mix, 1 dilution, and 10 recycle). Most of these were made and characterized in FY21. Taggant acceptability was based upon manufacturability, detectability, and persistence from the standpoint of two detection options: bulk chemical analysis (for “chemical taggants”) and microstructural analysis (for “second phase taggants”). Taggant detection in both up-front manufacturing and in the face of “degradations” such as dilution, mixing, and recycling was generally good. Two independent laboratories carried out chemical analysis on most of the castings, and often at several locations within a casting, and the results are discussed. Scanning electron microscopy+EDS microanalysis revealed the second phases mostly contained the expected tagging elements. The shapes and 2 spatial distributions of these micron-sized carbides, oxides, and intermetallic particles offers opportunities for further science-based investigation and tagging optimization. Overall, V and Co currently appear as the best choices for chemical taggants while Al, Ti, Mn, Co, Pd, and Tb all look good as second phase taggants. The other elements considered here – Sc, Ni, Ge, Nb, Ce, Ta, W, Ir, and Au – while not being ruled out, require more study to become viable options. It is of special note that in the recycling study only one of the 12 elements fell out of detection even after 10 meltings, demonstrating their persistence. An Appendix tabulates all chemical analysis results to enable more quantitative and statistical studies of detection opportunities and limitations, as a part of a related project.