ABSTRACT
Theoretical models for the coefficient of thermal expansion (CTE) first proposed in the 1970s are expanded upon, allowing them, for the first time, to be implemented over a wide temperature range. The models are of interest because they predict the effects of the changes in the crystal lattice spacing and crystallite modulus on the CTE. Hence, they can in turn be used to investigate the influence of pressure and irradiation on the CTE. To date, typographical and mathematical errors and incomplete or conflicting assumptions between the various papers had made the complex mathematical formulations difficult, if not impossible, to follow and apply. This paper has two main aims: firstly to revisit and review the CTE models, correcting the errors and compiling and updating various input data, secondly to use the revised models to investigate the effect of loading and irradiation on the CTE. In particular, the models have been applied to data for natural and highly orientated pyrolytic graphite and compared with experimental data, giving an insight into the influence of temperature, loading and irradiation on both single crystal and polycrystalline graphite. The findings lend credence to postulated microstructural mechanisms attributed to the in-reactor behaviour of nuclear graphite, which finds a wide use in predictive multiscale modelling.
ABSTRACT
This study has investigated the laboratory scale thermal oxidation of nuclear graphite, as a proof-of-concept for the treatment and decommissioning of reactor cores on a larger industrial scale. If showed to be effective, this technology could have promising international significance with a considerable impact on the nuclear waste management problem currently facing many countries worldwide. The use of thermal treatment of such graphite waste is seen as advantageous since it will decouple the need for an operational Geological Disposal Facility (GDF). Particulate samples of Magnox Reactor Pile Grade-A (PGA) graphite, were oxidised in both air and 60% O2, over the temperature range 400-1200°C. Oxidation rates were found to increase with temperature, with a particular rise between 700-800°C, suggesting a change in oxidation mechanism. A second increase in oxidation rate was observed between 1000-1200°C and was found to correspond to a large increase in the CO/CO2 ratio, as confirmed through gas analysis. Increasing the oxidant flow rate gave a linear increase in oxidation rate, up to a certain point, and maximum rates of 23.3 and 69.6 mg / min for air and 60% O2 respectively were achieved at a flow of 250 ml / min and temperature of 1000°C. These promising results show that large-scale thermal treatment could be a potential option for the decommissioning of graphite cores, although the design of the plant would need careful consideration in order to achieve optimum efficiency and throughput.
