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Radiochronometry provides the model age of nuclear materials, which is useful for understanding the production history of materials found outside of regulatory control. Certified reference materials (CRMs) are important for radiochronometry to increase confidence in measurement quality; however, the absence of 231Pa/235U CRMs necessitates that nuclear forensic laboratories measure the 231Pa/235U model ages of preexisting uranium reference materials. Here, new consensus 231Pa/235U model ages are reported from three nuclear forensic laboratories for three reference materials using current analytical methods. These updated consensus values can be used for quality control of 231Pa/235U model age measurements. [ABSTRACT FROM AUTHOR]

The isolation and purification of protactinium from uranium materials is essential for 231Pa–235U radiochronometry, but separating Pa from uranium-niobium alloys, a common material in the nuclear fuel cycle, is challenging due to the chemical similarity of Pa and Nb. Here we present three resin chromatography separation techniques for isolating Pa from U and Nb which were independently developed by three different laboratories through ad hoc adaptations of standard operating procedures. Our results underscore the need for and value of purification methods suitable for a diversity of uranium-based materials to ensure the operational readiness of nuclear forensics laboratories. [ABSTRACT FROM AUTHOR]

Radiochronometry analyses of three hydrolyzed UF6 gas samples were performed using the 230Th-234U and 231Pa-235U chronometers. All 230Th-234U model ages are younger than, and two of the three 231Pa-235U model ages overlap with, the known UF6 gas transfer dates. The 230Th-234U discordance is caused by 8–10% 230Th loss relative to the measurement reference date, likely during alkali hydrolysis. These results confirm that UF6 gas transfers effectively purify uranium from daughter progeny. Daughter progeny fractionation can occur if solutions are not kept within optimal conditions post-UF6 gas transfer and hydrolysis, and discordance between the 230Th-234U and 231Pa-235U chronometers may result from the laboratory procedures used to prepare samples. [ABSTRACT FROM AUTHOR]

The application of multiple radiochronometers in a forensic investigation of bulk uranium provides increased confidence for interpreting age-dating results. We have developed a streamlined method for the purification of Pa and Th from bulk uranium and have applied this method in analyzing uranium certified reference materials (CRMs) IRMM-1000 and CRM U100, using the 231Pa-235U and 230Th-234U radiochronometers. Our improved 233Pa spike calibration technique has replaced the time-intensive, conventional calibration using geologic rock standards. Paired Pa-U and Th-U age-dating analyses of CRM U100 produce concordant results. In contrast, analyses of IRMM-1000 demonstrate reproducibly-discordant Th-U and Pa-U age-dates. [ABSTRACT FROM AUTHOR]

A new determination of the 229Th half-life was made based on measurements of the 229Th massic activity of a high-purity solution for which the 229Th molality had previously been measured. The 229Th massic activity was measured by direct comparison with SRM 4328C using 4παβ liquid scintillation counting, NaI counting, and standard addition liquid scintillation counting. The massic activity was confirmed by isotope dilution alpha spectrometry measurements. The calculated 229Th half-life is (7825 ± 87) years (k = 2), which is shorter than the three most recent half-life determinations but is consistent with these values within uncertainties. [ABSTRACT FROM AUTHOR]

Data obtained from Sm-Nd and Rb-Sr isotopic measurements of lunar highlands' samples are renormalized to common standard values and then used to define ages with a common isochron regression algorithm. The reliability of these ages is evaluated using five criteria that include whether: (1) the ages are defined by multiple isotopic systems, (2) the data demonstrate limited scatter outside uncertainty, (3) initial isotopic compositions are consistent with the petrogenesis of the samples, (4) the ages are defined by an isotopic system that is resistant to disturbance by impact metamorphism, and (5) the rare-earth element abundances determined by isotope dilution of bulk of mineral fractions match those measured by in situ analyses. From this analysis, it is apparent that the oldest highlands' rock ages are some of the least reliable, and that there is little support for crustal ages older than approximately 4.40 Ga. A model age for ur- KREEP formation calculated using the most reliable Mg-suite Sm-Nd isotopic systematics, in conjunction with Sm-Nd analyses of KREEP basalts, is 4389 ± 45 Ma. This age is a good match to the Lu-Hf model age of 4353 ± 37 Ma determined using a subset of this sample suite, the average model age of 4353 ± 25 Ma determined on mare basalts with the 146Sm-142Nd isotopic system, with a peak in Pb-Pb ages observed in lunar zircons of approximately 4340 ± 20 Ma, and the oldest terrestrial zircon age of 4374 ± 6 Ma. The preponderance of ages between 4.34 and 4.37 Ga reflect either primordial solidification of a lunar magma ocean or a widespread secondary magmatic event on the lunar nearside. The first scenario is not consistent with the oldest ages reported for lunar zircons, whereas the second scenario does not account for concordance between ages of crustal rocks and mantle reservoirs. [ABSTRACT FROM AUTHOR]

Age dating of nuclear material can provide insight into source and suspected use in nuclear forensic investigations. We report here a method for the determination of the date of most recent chemical purification for uranium materials using the 235U-231Pa chronometer. Protactinium is separated from uranium and neptunium matrices using anion exchange resin, followed by sorption of Pa to an SiO2 medium. The concentration of 231Pa is measured by isotope dilution mass spectrometry using 233Pa spikes prepared from an aliquot of 237Np and calibrated in-house using the rock standard Table Mountain Latite and the uranium isotopic standard U100. Combined uncertainties of age dates using this method are 1.5 to 3.5 %, an improvement over alpha spectrometry measurement methods. Model ages of five uranium standard reference materials are presented; all standards have concordant 235U-231Pa and 234U-230Th model ages. [ABSTRACT FROM AUTHOR]

New Rb-Sr, (146,147)Sm-(142,143)Nd and Lu-Hf isotopic analyses of Mg-suite lunar crustal rocks 67667, 76335, 77215 and 78238, including an internal isochron for norite 77215, were undertaken to better define the time and duration of lunar crust formation and the history of the source materials of the Mg-suite. Isochron ages determined in this study for 77215 are: Rb-Sr=4450±270 Ma, (147)Sm-(143)Nd=4283±23 Ma and Lu-Hf=4421±68 Ma. The data define an initial (146)Sm/(144)Sm ratio of 0.00193±0.00092 corresponding to ages between 4348 and 4413 Ma depending on the half-life and initial abundance used for (146)Sm. The initial Nd and Hf isotopic compositions of all samples indicate a source region with slight enrichment in the incompatible elements in accord with previous suggestions that the Mg-suite crustal rocks contain a component of KREEP. The Sm/Nd-(142)Nd/(144)Nd correlation shown by both ferroan anorthosite and Mg-suite rocks is coincident with the trend defined by mare and KREEP basalts, the slope of which corresponds to ages between 4.35 and 4.45 Ga. These data, along with similar ages for various early Earth differentiation events, are in accord with the model of lunar formation via giant impact into Earth at ca 4.4 Ga., (© 2014 The Author(s) Published by the Royal Society. All rights reserved.)