-Uranium-series data for groundwater samples from the Nopal I uranium ore deposit were obtained to place constraints on radionuclide transport and hydrologic processes for a nuclear waste repository located in fractured, unsaturated volcanic tuff. Decreasing uranium concentrations for wells drilled in 2003 are consistent with a simple physical mixing model that indicates that groundwater velocities are low (~10 m/y). Uranium isotopic constraints, well productivities, and radon systematics also suggest limited groundwater mixing and slow flow in the saturated zone. Uranium isotopic systematics for seepage water collected in the mine adit show a spatial dependence which is consistent with longer water-rock interaction times and 2 higher uranium dissolution inputs at the front adit where the deposit is located. Uranium-series disequilibria measurements for mostly unsaturated zone samples indicate that 230 Th/ 238 U activity ratios range from 0.005-0.48 and 226 Ra/ 238 U activity ratios range from 0.006-113. 239 Pu/ 238 U mass ratios for the saturated zone are <2 × 10 -14 , and Pu mobility in the saturated zone is >1000 times lower than the U mobility. Saturated zone mobility decreases in the order 238 U~2 26 Ra > 230 Th~2 39 Pu. Radium and thorium appear to have higher mobility in the unsaturated zone based on U-series data from fractures and seepage water near the deposit.

Studies of uranium-series (U-series) disequilibria within and around ore deposits provide valuable information on the extent and timing of actinide mobility, via mineral-fluid interaction, over a range of spatial and temporal scales. Such information is useful in studies of analogs of high-level nuclear-waste repositories, as well as for mining and mineral extraction sites, locations of previous nuclear weapons testing, and legacy nuclear waste contamination. In this study we present isotope dilution mass spectrometry U-series measurements for fracture-fill materials (hematite, goethite, kaolinite, calcite, dolomite and quartz) from one such analog; the Nopal I uranium ore deposit situated at Peña Blanca in the Chihuahua region of northern Mexico. The ore deposit is located in fractured, unsaturated volcanic tuff and fracture-fill materials from surface fractures as well as fractures in a vertical drill core have been analyzed. High uranium concentrations in the fracture-fill materials (between 12 and 7700 ppm) indicate uranium mobility and transport from the deposit. Uranium concentrations generally decrease with horizontal distance away from the deposit but in this deposit there is no trend with depth below the surface. Isotopic activity ratios, 238 U-234 U-230 Th-232 Th linear age trends, and U-Th-Pa model ages indicate an actinide mobility evolution that can be characterized as complex and varied. There is evidence of both open and closed system behavior for uranium, depending on both sample and timescale. The 234 U/ 238 U activity ratios indicate U mobility from 1.2-0.2 Ma. In the last 0.2 Ma there is isotopic evidence for some U mobility but mostly U immobility. In almost all cases the Th-Pa radionuclides studied here have been immobile for the past 200 ka. Radium appears to have been recently (0.1-8 ka) mobile due to ongoing fluid flow in the fractures. Overall, the mainly closed system behavior for U-Th-Pa over the past ~200 ka provides an indicator of the geochemical immobility of these actinides over timescales relevant for potential nuclear waste repositories situated in fractured, unsaturated tuff.

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Recent advances in high-resolution, rapid, in situ microanalytical techniques present numerous opportunities for the analytical community, provided accurately characterized reference materials are available. Here, we present multicollector thermal ionization mass spectrometry (MC-TIMS) and multicollector inductively coupled plasma mass spectrometry (MC-ICP-MS) uranium and thorium concentration and isotopic data obtained by isotope dilution for a suite of newly available Chinese Geological Standard Glasses (CGSG) designed for microanalysis. These glasses exhibit a range of compositions including basalt, syenite, andesite, and a soil. Uranium concentrations for these glasses range from ∼2 to 14 μg g(-1), Th/U weight ratios range from ∼4 to 6, (234)U/(238)U activity ratios range from 0.93 to 1.02, and (230)Th/(238)U activity ratios range from 0.98 to 1.12. Uranium and thorium concentration and isotopic data are also presented for a rhyolitic obsidian from Macusani, SE Peru (macusanite). This glass can also be used as a rhyolitic reference material, has a very low Th/U weight ratio (around 0.077), and is approximately in (238)U-(234)U-(230)Th secular equilibrium. The U-Th concentration data agree with but are significantly more precise than those previously measured. U-Th concentration and isotopic data agree within estimated errors for the two measurement techniques, providing validation of the two methods. The large (238)U-(234)U-(230)Th disequilibria for some of the glasses, along with the wide range in their chemical compositions and Th/U ratios should provide useful reference points for the U-series analytical community.