Publications

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Spent nuclear fuel contains 129I, which is of particular concern due to its very long half-life, its potential mobility in the environment, and its deleterious effect on human health. In spent fuel reprocessing schemes under consideration, a gas stream containing 129I2 would be passed through a bed of Ag-loaded zeolites such as Ag-mordenite (Ag-MOR). We have investigated the use of a low-temperature sintering bismuth-silicon-zinc- oxide glass powder mixed with either AgI or AgI-MOR to produce dense glass composite material waste forms that can be processed at 550°C, where AgI volatility is low. We have demonstrated that when fine silver flake is added to the mixture, any adsorbed I2 released during heating of AgI-MOR reacts with the silver to form AgI in situ. Furthermore, we have shown that mixtures of the glass with the AgI-MOR or AgI are durable in aqueous environments. Finally, we have developed a process to fabricate core/shell waste forms where the core of AgI-MOR or AgI and glass is encased in a shell of glass that protects the core from contact with the environment. To prevent cracking of the shell due to thermal expansion mismatch between the core and shell, amorphous silica was added to the shell to form a composite with a lower coefficient of thermal expansion. © 2011 The American Ceramic Society.

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We report on the novel room temperature method of synthesizing advanced nuclear fuels; a method that virtually eliminates any volatility of components. This process uses radiolysis to form stable nanoparticle (NP) nuclear transuranic (TRU) fuel surrogates and in-situ heated stage TEM to sinter the NPs. The radiolysis is performed at Sandia's Gamma Irradiation Facility (GIF) 60Co source (3 x 10{sup 6} rad/hr). Using this method, sufficient quantities of fuels for research purposes can be produced for accelerated advanced nuclear fuel development. We are focused on both metallic and oxide alloy nanoparticles of varying compositions, in particular d-U, d-U/La alloys and d-UO2 NPs. We present detailed descriptions of the synthesis procedures, the characterization of the NPs, the sintering of the NPs, and their stability with temperature. We have employed UV-vis, HRTEM, HAADF-STEM imaging, single particle EDX and EFTEM mapping characterization techniques to confirm the composition and alloying of these NPs.

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Reprocessing nuclear fuel releases gaseous radio-iodine containing compounds which must be captured and stored for prolonged periods. Ag-loaded mordenites are the leading candidate for scavenging both organic and inorganic radioiodine containing compounds directly from reprocessing off gases. Alternately, the principal off-gas contaminant, I2, and I-containing acids HI, HIO3, etc. may be scavenged using caustic soda solutions, which are then treated with bismuth to put the iodine into an insoluble form. Our program is focused on using state-of-the-art materials science technologies to develop materials with high loadings of iodine, plus high long-term mechanical and thermal stability. In particular, we present results from research into two materials areas: (1) zeolite-based separations and glass encapsulation, and (2) in-situ precipitation of Bi-I-O waste forms. Ag-loaded mordenite is either commercially available or can be prepared via a simple Ag+ ion exchange process. Research using an Ag+-loaded Mordenite zeolite (MOR, LZM-5 supplied by UOP Corp.) has revealed that I2 is scavenged in one of three forms, as micron-sized AgI particles, as molecular (AgI)x clusters in the zeolite pores and as elemental I2 vapor. It was found that only a portion of the sorbed iodine is retained after heating at 95o C for three months. Furthermore, we show that even when the Ag-MOR is saturated with I2 vapor only roughly half of the silver reacted to form stable AgI compounds. However, the Iodine can be further retained if the AgI-MOR is then encapsulated into a low temperature glass binder. Follow-on studies are now focused on the sorption and waste form development of Iodine from more complex streams including organo-iodine compounds (CH3I). Bismuth-Iodate layered phases have been prepared from caustic waste stream simulant solutions. They serve as a low cost alternative to ceramics waste forms. Novel compounds have been synthesized and solubility studies have been completed using competing groundwater anions (HCO3-, Cl- and SO42-). Distinct variations in solubility were found that related to the structures of the materials.

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Inelastic neutron scattering, density functional theory, ab initio molecular dynamics, and classical molecular dynamics were used to examine the behavior of nanoconfined water in palygorskite and sepiolite. These complementary methods provide a strong basis to illustrate and correlate the significant differences observed in the spectroscopic signatures of water in two unique clay minerals. Distortions of silicate tetrahedra in the smaller-pore palygorskite exhibit a limited number of hydrogen bonds having relatively short bond lengths. In contrast, without the distorted silicate tetrahedra, an increased number of hydrogen bonds are observed in the larger-pore sepiolite with corresponding longer bond distances. Because there is more hydrogen bonding at the pore interface in sepiolite than in palygorskite, we expect librational modes to have higher overall frequencies (i.e., more restricted rotational motions); experimental neutron scattering data clearly illustrates this shift in spectroscopic signatures. Distortions of the silicate tetrahedra in these minerals effectively disrupts hydrogen bonding patterns at the silicate-water interface, and this has a greater impact on the dynamical behavior of nanoconfined water than the actual size of the pore or the presence of coordinatively-unsaturated magnesium edge sites.