The evaporation of a range of synthetic pore water solutions representative of the potential high-level-nuclear-waste repository at Yucca Mountain, NV is being investigated. The motivation of this work is to understand and predict the range of brine compositions that may contact the waste containers from evaporation of pore waters, because these brines could form corrosive thin films on the containers and impact their long-term integrity. A relatively complex synthetic Topopah Spring Tuff pore water was progressively concentrated by evaporation in a closed vessel, heated to 95 C in a series of sequential experiments. Periodic samples of the evaporating solution were taken to determine the evolving water chemistry. According to chemical divide theory at 25 C and 95 C our starting solution should evolve towards a high pH carbonate brine. Results at 95 C show that this solution evolves towards a complex brine that contains about 99 mol% Na{sup +} for the cations, and 71 mol% Cl{sup -}, 18 mol% {Sigma}CO{sub 2}(aq), 9 mol%SO{sub 4}{sup 2-} for the anions. Initial modeling of the evaporating solution indicates precipitation of aragonite, halite, silica, sulfate and fluoride phases. The experiments have been used to benchmark the use of the EQ3/6 geochemical code in predicting the evolution of carbonate-rich brines during evaporation.

The proposed Repository presents a familiar materials performance application that is regularly encountered in energy, transportation and other industries. The widely accepted approach to dealing with materials performance is to identify the performance requirements, to determine the operating conditions to which materials will be exposed and to select materials of construction that perform well in those conditions. A special feature of the proposed Yucca Mountain Repository is the extremely long time frame of interest, i.e. 10,000's of years and longer. Thus, the time evolution of the environment in contact with waste package surfaces and the time evolution of corrosion damage that may result are of primary interest in the determination of expected performance. An approach is presented to the analysis of localized corrosion during a time period when it is possible for waters from drips and seepage to contact the waste package surfaces, and the analysis is demonstrated for the water chemistry of mixed salt solutions and a set of time-temperature-relative humidity profiles for a hot, mid and cool temperature waste package. Based on the analysis, there are large time periods when localized corrosion can not be supported, and no corrosion damage will occur. Further analysis can then focus on time periods when it is possible for localized corrosion to occur and the determination of the evolution of any corrosion damage.

In these experiments we studied the behavior of a synthetic concentrated J13 solution as it comes in contact with a Ni-Cr-Mo-alloy selected for waste canisters in the designated high-level nuclear-waste repository at Yucca Mountain, Nevada. Concentrated synthetic J13 solution was allowed to drip slowly onto heated test specimens (90 C, 60% relative humidity) where the water moved down the surface of the specimens, evaporated and minerals precipitated. Mineral separation or zoning along the evaporation path was not observed. We infer from solid analyses and geochemical modeling, that the most corrosive components (Ca, Mg, and F) are limited by mineral precipitation. Minerals identified by x-ray diffraction include thermonatrite, natrite, and trona, all sodium carbonate minerals, as well as kogarkoite (Na{sub 3}SO{sub 4}F), halite (NaCl), and niter (KNO{sub 3}). Calcite and a magnesium silicate precipitation are based on chemical analyses of the solids and geochemical modeling. The most significant finding of this study is that sulfate and fluoride concentrations are controlled by the solubility of kogarkoite. Kogarkoite thermodynamic data are needed in the Yucca Mountain Project database to predict the corrosiveness of carbonate brines and to establish the extent to which fluoride is removed from the brines as a solid.

This paper describes the focusing horn system for the proposed very long baseline neutrino oscillation experiment using a neutrino beam from BNL to an underground facility such as the Homestake Mine in South Dakota. The proposed experiment uses a 1 MW upgraded AGS. In order to achieve this performance the AGS will operate with a cycle time of 2.5 Hz and 8.9 x 10{sup 13} protons on target at 28 GeV. This paper discusses the design criteria of a horn system necessary to handle this intense beam and the optical geometry to achieve the desired flux distribution at the detector.

Synchrotron X-ray absorption spectroscopy (XAS) is one of the few techniques that can supply molecular-scale information for a variety of elements at concentrations relevant to natural systems in non-vacuum conditions. Bulk XAS analysis supplies the dominant chemical bonding mode(s) for a specific element. In complex materials such as natural soils and sediments, however, the dominant mode may not necessarily be the most reactive because changes in speciation at surfaces may results in changes in reactivity. Our previous work at Naval Air Station (NAS) Alameda (CA) focused on in situ metal chemistry in surface and deep sediments, and the impact of metal mobility by sediment oxidation. Estuary sediments at the Alameda Naval Station Air in California have elevated metal concentrations that increase with increasing depth. The metal concentrations in these sediments are: Cd (10-350 ppm), Cr (200-1000 ppm), Cu (100-230 ppm), Pb (200-1200 ppm) and Zn (250-600 ppm). We have extensively characterized these sediments using bulk XAS and other non-synchrotron supporting methods [1]. In this experiment, we collected fluorescence element maps using synchrotron X-ray microprobe of unreacted and seawater-oxidized sediment samples from Alameda NAS to determine the spatial distribution and correlation of lead, zinc, and iron. We then compared micro-XANES spectra for lead and zinc collected with the X-ray microprobe to previously collected bulk XANES spectra. The results from our bulk XAS characterization of the sediments showed both oxide and sulfide components for the trace metals. However, the bulk XAS data were not able to identify the composition of the oxide component (i.e. carbonate or hydroxide), nor could absorbed species or solid solutions be definitively identified. Our objective in using micro-XANES and fluorescence element maps was to attempt a more precise identification of metal speciation in or on individual particles.