Abstract
Triuranium disilicide (U3Si2) fuel with silicon carbide (SiC) composite cladding is being considered as an advanced concept/accident tolerant fuel for light water reactors thus, understanding their chemical compatibility under operational and accident conditions is paramount. Here we provide a comprehensive view of the interaction between U3Si2 and SiC by utilizing density functional theory calculations supported by diffusion couple experiments. From the calculated reaction energies, we demonstrate that triuranium pentasilicide (U3Si5), uranium carbide (UC), U20Si16C3, and uranium silicide (USi) phases can form at the interface. A detailed study of U3Si2 and SiC defect formation energies of the equilibrated materials yielding the interfacial phases U20Si16C3, U3Si5 and UC reveal a thermodynamic driving force for generating defects in both fuel and cladding. The absence of either the U3Si2 or SiC phase, however, causes the defect formation energies in the other phase to be positive, removing the driving force for additional interfacial reactions. The diffusion couple experiments confirm the conclusion with demonstrated restricted formation of U3Si5, UC, and U20Si16C3/USi phases at the interface. The resulting lack of continuous interaction between the U3Si2 and SiC, reflects the diminishing driving force for defect formation, demonstrating the substantial stability of this fuel-cladding system.