Molybdenum isotope fractionation in uranium oxides and during key processes of the nuclear fuel cycle: Towards a new nuclear forensic tool

Abstract

The ability to identify the sources of nuclear materials using various analytical methods has become a major target of nuclear forensics science. However, despite the emergence of novel tools developed in recent years, it has become obvious that accurate identification of sources requires multiple tools. Here, we have developed a new isotope tool based on Mo isotopes that could be used in nuclear forensics. Molybdenum is a trace element that is found in significant levels in uranium ores (0.5–4800 ppm), uranium minerals (0.02–6000 ppm) and uranium ore concentrates (UOCs, from 0.7 to 1400 ppm). The Mo isotope composition, reported as δ98Mo was analyzed in these materials and shown to have a significant variability from −2.62 to +0.30‰ in uranium ores and from −3.50 to +0.46‰ in UOCs. In uranium ores, the largest Mo isotope fractionation is found in deposits of sedimentary origin while the few ores with a magmatic origin show limited Mo isotope fractionation. Thus, the Mo isotope ratios may ultimately be used to distinguish high temperature from low temperature uranium ores. The δ98Mo values in UOCs also show a significant range that not only originate from variations in ore compositions but can also be attributed to ore processing such as leaching, solvent extraction, resin extraction and UOC precipitation. Laboratory experiments based on existing protocols of uranium ore separation demonstrate the existence of sizeable Mo isotope fractionation associated with these processes. Experiments with solvent extraction and precipitation of ammonium diuranate and peruranate show that the refined uranium fraction is enriched in light Mo isotopes in both cases. In the case of a uranium ore (SOMAÏR, Niger) and associated UOC, the observed fractionation can possibly be assigned to the combined effect of solvent extraction and precipitation, although Mo isotope variability in ores and UOCs may make such a diagnostic difficult. Ultimately, these experiments can be used to reconstruct the Mo isotope composition of the ore, if there is sufficient knowledge about the ore processing flowsheet or to provide information about the type of uranium ore. Alternatively, it could be used to identify the process used for manufacturing a given UOC, if one can make an estimate about the composition of the ore, probably in conjunction with other tools. Our study demonstrates the potential of Mo isotopes as a useful tool in the field of nuclear forensics.