Isotopic Compositions of Uranium Reference Materials

Uranium isotopic compositions of a variety of U standard materials were measured at Lawrence Livermore National Laboratory and are reported here. Both thermal ionization mass spectrometry (TIMS) and multi-collector inductively couple plasma mass spectrometry (MC-ICPMS) were used to determine ratios of the naturally occurring isotopes of U. Establishing an internally coherent set of isotopic values for a range of U standards is essential for inter-laboratory comparison of small differences in 238U/235U, as well as the minor isotopes of U. Differences of ~1.3‰ are now being observed in 238U/235U in natural samples, and may play an important role in understanding U geochemistry where tracing the origin of U is aided by U isotopic compositions. The 238U/235U ratios were measured with a TRITON TIMS using a mixed 233U-236U isotopic tracer to correct for instrument fractionation. This tracer was extremely pure and resulted in only very minor corrections on the measured 238U/235U ratios of ~0.03. The values obtained for 238U/235U are: IRMM184 = 137.698 ± 0.020 (n=15), SRM950a = 137.870 ± 0.018 (n=8), and CRM112a = 137.866 ± 0.030 (n=16). Uncertainties represent 2 s.d. of the population. Our measured value for IRMM184 is in near-perfect agreement with the certified value of 137.697 ± 0.042. However, the U isotopic compositions of SRM950a and CRM112a are not certified. Minor isotopes of U were determined with a Nu Plasma HR MC-ICPMS and mass bias was corrected by sample/standard bracketing to IRMM184, using its certified 238U/235U ratio. Thus, the isotopic compositions determined using both instruments are compatible. The values obtained for 234U/235U are: SRM950a = (7.437 ± 0.043)x10-3 (n=18), and CRM112a = (7.281 ± 0.050)x10-3 (n=16), both of which are in good agreement with published values. The value for 236U/235U in SRM950a was determined to be (8.48 ± 2.63)x10-6, whereas 236U was not detected in CRM112a. We are currently obtaining the U isotopic composition of CRM129a. Preliminary results suggest that the 238U/235U ratio is within error, but slightly lower than the certified value of 137.71.