The nickel-plated zircaloy-4 is used as a tritium (3H) getter in the tritium-producing burnable absorber rods (TPBARs) to capture 3H produced in the 6Li-riched annular γ-LiAlO2 pellet under neutron irradiation. The experimental data and our previous theoretical results showed that the 3H species produced from the γ-LiAlO2 pellet were mainly 3H2 and 3H2O. These 3H species diffuse from the surface of the LiAlO2 pellet across vacuum to the nickel-plated zircaloy-4 getter and then further diffuse into the getter to chemically form metal hydrides. While a number of studies show that oxygen binds strongly as compared to 3H on the nickel (Ni) layer, the detailed mechanism of 3H species absorption and diffusion across the Ni plate and Ni/Zr interface are still unclear. By employing density functional theory calculations, here we explored the 3H2 and 3H2O species adsorption and dissociation on the Ni(111) surface and diffusion into the Ni sublayer. Our results indicated that the 3H2 and 3H2O dissociate on the Ni(111) surface. The NiOx and Ni(O3H)x could be formed in the Ni layer due to the higher oxygen (O) diffusion energy barrier and formation of Ni vacancy defects. The oxygen was found to be retained in the Ni layer from diffusing across the Ni-Zr interface. This was revealed by comparing the diffusion barriers for 3H with O. 3H was found to have nearly three times smaller diffusion barrier than for O, making 3H comparatively easier to diffuse through the Ni layer. The obtained results provide guidelines for experimental measurements on 3H retention behavior in TPBARs and may open further avenues to explore the impurity effects on 3H diffusion and storage at the Ni/zircaloy interfaces.
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