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Parker, Stephen Scott
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report
Molybdenum Disilicide Oxidation Kinetics in High Temperature Steam
Abstract
The Fuel Cycle Research and Development program’s Advanced Fuels Campaign is currently supporting a range of experimental efforts aimed at the development and qualification of ‘accident tolerant’ nuclear fuel forms. One route to enhance the accident tolerance of nuclear fuel is to replace the zirconium alloy cladding, which is prone to rapid oxidation in steam at elevated temperatures, with a more oxidation-resistant cladding. Several cladding replacement solutions have been envisaged. The cladding can be completely replaced with a more oxidation resistant alloy, a layered approach can be used to optimize the strength, creep resistance, and oxidation tolerance of various materials, or the existing zirconium alloy cladding can be coated with a more oxidation-resistant material. Molybdenum is one candidate cladding material favored due to its high temperature creep resistance. However, it performs poorly under autoclave testing and suffers degradation under high temperature steam oxidation exposure. Development of composite cladding architectures consisting of a molybdenum core shielded by a molybdenum disilicide (MoSi<sub>2</sub>) coating is hypothesized to improve the performance of a Mo-based cladding system. MoSi<sub>2</sub> was identified based on its high temperature oxidation resistance in O<sub>2</sub> atmospheres (e.g. air and “wet air”). However, its behavior in H<sub>2</sub>O is less known. This report presents thermogravimetric analysis (TGA), scanning electron microscopy (SEM), and x-ray diffraction (XRD) results for MoSi<sub>2</sub> exposed to 670-1498 K water vapor. Synthetic air (80-20%, Ar-O<sub>2</sub>) exposures were also performed, and those results are presented here for a comparative analysis. It was determined that MoSi<sub>2</sub> displays drastically different oxidation behavior in water vapor than in dry air. In the 670-1498 K temperature range, four distinct behaviors are observed. Parabolic oxidation is exhibited in only 670-773 K water vapor, a temperature range in which the material pests in dry O<sub>2</sub> environments. From 877-1084 K in water vapor, MoSi<sub>2</sub> undergoes rapid mass gain resulting in oxidation throughout the bulk of the sample at 980 K and 1084 K. The resulting material displays swelling and warping after the 980-1084 K exposures. A pre-passivation heat treatment performed at 1395 K was found capable of producing a coarse SiO<sub>2</sub> layer that limited pesting at lower temperatures in water vapor over the time periods investigated.