Publications

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This report summarizes the work completed under the Laboratory Directed Research and Development (LDRD) project 09-1351, 'Computational Investigation of Thermal Gas Separation for CO{sub 2} Capture'. Thermal gas separation for a binary mixture of carbon dioxide and nitrogen is investigated using the Direct Simulation Monte Carlo (DSMC) method of molecular gas dynamics. Molecular models for nitrogen and carbon dioxide are developed, implemented, compared to theoretical results, and compared to several experimental thermophysical properties. The molecular models include three translational modes, two fully excited rotational modes, and vibrational modes, whose degree of excitation depends on the temperature. Nitrogen has one vibrational mode, and carbon dioxide has four vibrational modes (two of which are degenerate). These models are used to perform a parameter study for mixtures of carbon dioxide and nitrogen confined between parallel walls over realistic ranges of gas temperatures and nominal concentrations of carbon dioxide. The degree of thermal separation predicted by DSMC is slightly higher than experimental values and is sensitive to the details of the molecular models.

Understanding the corrosion of spent nuclear fuel (SNF) and the subsequent mobilization of released radionuclides, particularly under oxidizing conditions, is one of the key issues in evaluating the long-term performance of a nuclear waste repository. However, the large amounts of iron in the metal waste package may create locally reducing conditions that would lower corrosion rates for the SNF, as well as reduce the solubility of some key radionuclides, e.g., Tc and Np. In order to investigate the interactions among SNF-waste package-fluids, four smallscale (∼1:40 by length) waste package mockups were constructed using metals similar to those proposed for use in waste packages at the proposed repository at Yucca Mountain. Each mockup experiment differed with respect to water input, exposure to the atmosphere, and temperature. Simulated Yucca Mountain process water (YMPW) was injected into three of the mockups at a rate of 200 μL per day for five days a week using a calibrated needle syringe. The YMPW was prepared by equilibrating 50 mg/L silica as sodium metasilicate with air, and adding enough HC1 to lower the pH to 7.6 in contact with an excess of powdered calcite. X-ray powder diffraction and scanning electron microscopy confirm that, where corrosion occurred, the dominant corrosion product in all cases was magnetite. In the high temperature (60°C) experiment, hematite and a fibrous, Fe-O-Cl phase were also identified. The Fe(II)/Fe(III) ratios measured in the corrosion products using a wet chemistry technique indicate extremely low oxygen fugacities (10-36 bar). Experiments are in progress in which 0.1g powdered UO2 was included in the mock-up in order to investigate the relative kinetics of Fe and U oxidation and to identify the U corrosion products formed under these conditions. © 2008 Materials Research Society.

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Potentially corrosive brines can form during post-closure by deliquescence of salt minerals in dust deposited on the surface of waste packages at Yucca Mountain during operations and the pre-closure ventilation period. Although thermodynamic modeling and experimental studies of brine deliquescence indicates that brines are likely to form, they will be nitrate-rich and non-corrosive. Processes that modify the brines following deliquescence are beneficial with respect to inhibition of corrosion. For example, acid degassing (HCl, HNO3) could dry out brines, but kinetic limitations are likely to limit the effect to increasing their passivity by raising the pH and increasing the NO3/Cl ratio. Predicted dust quantities and maximum brine volumes on the waste package surface are small, and physical isolation of salt minerals in the dust may inhibit formation of eutectic brines and decrease brine volumes. If brines do contact the WP surface, small droplet volumes and layer thicknesses do not support development of diffusive gradients necessary for formation on separate anodic-cathodic zones required for localized corrosion. Finally, should localized corrosion initiate, corrosion product buildup will stifle corrosion, by limiting oxygen access to the metal surface, by capillary retention of brine in corrosion product porosity, or by consumption of brine components (Cl-). © 2006 Materials Research Society.

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