Jake W. McMurray

Carbothermic Synthesis of ~820- m UN Kernels. Investigation of Process Variables

This report details the continued investigation of process variables involved in converting sol-gel-derived, urainia-carbon microspheres to ~820-μm-dia. UN fuel kernels in flow-through, vertical refractory-metal crucibles at temperatures up to 2123 K. Experiments included calcining of air-dried UO3-H2O-C microspheres in Ar and H2-containing gases, conversion of the resulting UO2-C kernels to dense UO2:2UC in the same gases and vacuum, and its conversion in N2 to in UC1-xNx. The thermodynamics of the relevant reactions were applied extensively to interpret and control the process variables. Producing the precursor UO2:2UC kernel of ~96% theoretical density was required, but its subsequent conversion to UC1-xNx at 2123 K was not accompanied by sintering and resulted in ~83-86% of theoretical density. Decreasing the UC1-xNx kernel carbide component via HCN evolution was shown to be quantitatively consistent with present and past experiments and the only useful application of H2 in the entire process.

M3FT-15OR0202212: SUBMIT SUMMARY REPORT ON THERMODYNAMIC EXPERIMENT AND MODELING

Modeling the behavior of nuclear fuel with a physics-based approach uses thermodynamics for key inputs such as chemical potentials and thermal properties for phase transformation, microstructure evolution, and continuum transport simulations. Many of the lanthanide (Ln) elements and Y are high-yield fission products. The U-Y-O and U-Ln-O ternaries are therefore key subsystems of multi-component high-burnup fuel. These elements dissolve in the dominant urania fluorite phase affecting many of its properties. This work reports on an effort to assess the thermodynamics of the U-Pr-O and U-Y-O systems using the CALPHAD (CALculation of PHase Diagrams) method. The models developed within this framework are capable of being combined and extended to include additional actinides and fission products allowing calculation of the phase equilibria, thermochemical and material properties of multicomponent fuel with burnup.