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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Radioactive iodine, 129I, a component of spent nuclear fuel, is of particular concern due to its extremely long half-life, its potential mobility in the environment and its effects on human health. In the spent fuel reprocessing scheme under consideration, the 129I is released in gaseous form and collected using Ag-loaded zeolites such as Ag-mordenite. The 129I can react with the Ag to form insoluble AgI. We have investigated the use of low temperature-sintering glass powders mixed with either AgI or AgI-zeolite to produce dense waste forms that can be processed at 500°C, where AgI volatility is low. These mixtures can contain up to 20 wt% crushed AgI-mordenite or up to 50 wt% AgI. Both types of waste forms were found to have the high iodine leach resistance in these initial studies.

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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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