Diffusion Behavior of Oversized Fission Products in bcc Fe Cladding: A First-Principles Study

Fuel-Cladding Chemical Interaction (FCCI) poses significant challenges in nuclear reactors, where fission products from nuclear fuel interact with Fe-based cladding materials, potentially compromising their structural integrity. This study investigates the diffusion behavior of oversized fission products, Pr, Nd, Ce, and La, within bcc Fe cladding using density functional theory (DFT), nudged elastic band (NEB) method, and self-consistent mean field (SCMF) theory. Our results reveal significant long-range vacancy binding energies, particularly up to the 6th nearest neighbor, with La exhibiting the strongest binding affinity, followed by Nd, Ce, and Pr. The NEB calculations indicate significant high barriers for the dissociation of 1nn vacancy-solute pairs for all fission products. The tracer diffusion coefficients of these fission products was derived in Arrhenius form. The significant trapping effect of vacancies by a very dilute amount of fission products reduces vacancy mobility, leading to an oversaturation of point defects, void nucleation, and swelling. These are critical issues for irradiated cladding materials. The tracer diffusion coefficients indicate that Nd diffuses the fastest, followed by La, Ce, and Pr. This study provides essential insights for developing advanced cladding materials and design strategies to mitigate FCCI, ultimately enhancing nuclear reactor safety and performance.. Authors: Ke, Jia-Hong [Idaho National Laboratory (INL), Idaho Falls, ID (United States)] (ORCID:0000000289317885); Song, Rongjie [Idaho National Laboratory (INL), Idaho Falls, ID (United States)] (ORCID:0009000790378654). DOE Contract: AC07-05ID14517. Subjects: 11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS; 36 MATERIALS SCIENCE; 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; Cladding materials; Density functional theory; diffusion model; fission products; oversized atoms; vacancy-solute binding