Hanford sediments impacted by hyperalkaline high level radioactive waste have undergone incongruent silicate mineral weathering concurrent with contaminant uptake. In this project, we studied the impact of background pore water (BPW) on strontium, cesium and iodine desorption and transport in Hanford sediments that were experimentally weathered by contact with simulated hyperalkaline tank waste leachate (STWL) solutions. Using those lab-weathered Hanford sediments (HS) and model precipitates formed during nucleation from homogeneous STWL solutions (HN), we (i) provided thorough characterization of reaction products over a matrix of field-relevant gradients in contaminant concentration, partial pressure of carbon dioxide, and reaction time; (ii) improved molecular-scale understanding of how sorbate speciation controls contaminant desorption from weathered sediments upon removal of caustic sources; and (iii) developed a mechanistic, predictive model of meso- to field-scale contaminant reactive transport under these conditions. In this final report, we provide detailed descriptions of our results from this three-year study, completed in 2012 following a one-year no cost extension.

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The main purpose of this project was to improve the fundamental mechanistic understanding and quantification of long-term colloid mobilization and colloid-facilitated transport of radionuclides in the vadose zone, with special emphasis on the semi-arid Hanford site. While we focused some of the experiments on hydrogeological and geochemical conditions of the Hanford site, many of our results apply to colloid and colloid-facilitated transport in general. Specific objectives were (1) to determine the mechanisms of colloid mobilization and colloid-facilitated radionuclide transport in undisturbed Hanford sediments under unsaturated flow, (2) to quantify in situ colloid mobilization and colloid-facilitated radionuclide transport from Hanford sediments under field conditions, and (3) to develop a field-scale conceptual and numerical model for colloid mobilization and transport at the Hanford vadose zone, and use that model to predict long-term colloid and colloid- facilitated radionuclide transport. To achieve these goals and objectives, we have used a combination of experimental, theoretical, and numerical methods at different spatial scales, ranging from microscopic investigations of single particle attachment and detachment to larger-scale field experiments using outdoor lysimeters at the Hanford site. Microscopic and single particle investigations provided fundamental insight into mechanisms of colloid interactions with the air-water interface. We could show that a …

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Durability testing was performed on an external fuel processor (EFP) for a solid oxide fuel cell (SOFC) power plant. The EFP enables the SOFC to reach high system efficiency (electrical efficiency up to 60%) using pipeline natural gas and eliminates the need for large quantities of bottled gases. LG Fuel Cell Systems Inc. (formerly known as Rolls-Royce Fuel Cell Systems (US) Inc.) (LGFCS) is developing natural gas-fired SOFC power plants for stationary power applications. These power plants will greatly benefit the public by reducing the cost of electricity while reducing the amount of gaseous emissions of carbon dioxide, sulfur oxides, and nitrogen oxides compared to conventional power plants. The EFP uses pipeline natural gas and air to provide all the gas streams required by the SOFC power plant; specifically those needed for start-up, normal operation, and shutdown. It includes a natural gas desulfurizer, a synthesis-gas generator and a start-gas generator. The research in this project demonstrated that the EFP could meet its performance and durability targets. The data generated helped assess the impact of long-term operation on system performance and system hardware. The research also showed the negative impact of ambient weather (both hot and cold conditions) on system operation …

Improving the representation of local and non-local aerosol interactions in state-of-the-science regional climate models is a priority for the coming decade (Zhang, 2008). With this aim in mind, we have combined two new technologies that have a useful synergy: (1) an aerosol-enabled regional climate model (Advanced Weather Research and Forecasting Model with Chemistry WRF-Chem), whose primary weakness is a lack of high quality boundary conditions and (2) an aerosol-enabled multiscale modeling framework (PNNL Multiscale Aerosol Climate Model (MACM)), which is global but captures aerosol-convection-cloud feedbacks, and thus an ideal source of boundary conditions. Combining these two approaches has resulted in an aerosol-enabled modeling framework that not only resolves high resolution details in a particular region, but crucially does so within a global context that is similarly faithful to multi-scale aerosol-climate interactions. We have applied and improved the representation of aerosol interactions by evaluating model performance over multiple domains, with (1) an extensive evaluation of mid-continent precipitation representation by multiscale modeling, (2) two focused comparisons to transport of aerosol plumes to the eastern United States for comparison with observations made as part of the International Consortium for Atmospheric Research on Transport and Transformation (ICARTT), with the first being idealized and the …

The three major components of this research were: 1. Application of minimally invasive, cost effective hydrogeophysical techniques (surface and borehole), to generate fine scale (~1m or less) 3D estimates of subsurface heterogeneity. Heterogeneity is defined as spatial variability in hydraulic conductivity and/or hydrolithologic zones. 2. Integration of the fine scale characterization of hydrogeologic parameters with the hydrogeologic facies to upscale the finer scale assessment of heterogeneity to field scale. 3. Determination of the relationship between dual-domain parameters and practical characterization data.

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