Neptunium Transport Behavior in the Vicinity of Underground Nuclear Tests at the Nevada Test Site

[摘要] We used short lived {sup 239}Np as a yield tracer and state of the art magnetic sector ICP-MS to measure ultra low levels of {sup 237}Np in a number of 'hot wells' at the Nevada National Security Site (NNSS), formerly known as the Nevada Test Site (NTS). The results indicate that {sup 237}Np concentrations at the Almendro, Cambric, Dalhart, Cheshire and Chancellor sites, are in the range of 3 x 10{sup -5} to 7 x 10{sup -2} pCi/L and well below the MCL for alpha emitting radionuclides (15 pCi/L) (EPA, 2009). Thus, while Np transport is believed to occur at the NNSS, activities are expected to be well below the regulatory limits for alpha-emitting radionuclides. We also compared {sup 237}Np concentration data to other radionuclides, including tritium, {sup 14}C, {sup 36}Cl, {sup 99}Tc, {sup 129}I, and plutonium, to evaluate the relative {sup 237}Np transport behavior. Based on isotope ratios relative to published unclassified Radiologic Source Terms (Bowen et al., 1999) and taking into consideration radionuclide distribution between melt glass, rubble and groundwater (IAEA, 1998), {sup 237}Np appears to be substantially less mobile than tritium and other non-sorbing radionuclides, as expected. However, this analysis also suggests that {sup 237}Np mobility is surprisingly similar to that of plutonium. The similar transport behavior of Np and Pu can be explained by one of two possibilities: (1) Np(IV) and Pu(IV) oxidation states dominate under mildly reducing NNSS groundwater conditions resulting in similar transport behavior or (2) apparent Np transport is the result of transport of its parent {sup 241}Pu and {sup 241}Am isotopes and subsequent decay to {sup 237}Np. Finally, measured {sup 237}Np concentrations were compared to recent Hydrologic Source Term (HST) models. The 237Np data collected from three wells in Frenchman Flat (RNM-1, RNM-2S, and UE-5n) are in good agreement with recent HST transport model predictions (Carle et al., 2005). The agreement provides confidence in the results of the predictive model. The comparison to Cheshire HST model predictions (Pawloski et al, 2001) is somewhat ambiguous due to the low concentration resolution of the particle transport model.

[发布日期] 2010-12-03 [发布机构] Lawrence Livermore National Laboratory

[关键词] Source Terms;Decay;Neptunium 239;Isotope Ratio;Neptunium