Design, structural characterization, and simulated radiation-transport assessment of high-entropy (GdErSmEuYb)2X2O7 (X = Hf, Zr, Ce, Si) rare-earth oxides

This study investigates the structural, microstructural, surface-chemical, and radiation attenuation behaviour of high-entropy rare-earth oxide (HEO) powder compositions synthesized as TBC-related candidate coating materials, whose radiation attenuation potential was assessed within a computational Inconel-718-based sandwich model. Four compositions, namely (GdErSmEuYb)₂Hf₂O₇, (GdErSmEuYb)₂Ce₂O₇, (GdErSmEuYb)₂Zr₂O₇, and (GdErSmEuYb)₂Si₂O₇, were synthesized via high-energy ball milling followed by calcination at 1200 °C. X-ray diffraction results revealed the formation of distinct crystal structures depending on B-site chemistry, including defective fluorite and silicate-type phases. SEM-EDS mapping confirmed homogeneous elemental distribution, while XPS analysis demonstrated mixed valence states and different oxygen vacancy concentrations across the compositions. To evaluate radiation attenuation performance, a sandwich-type geometry consisting of a 10 mm Inconel-718 core with symmetrically defined simulated HEO layers was modelled using Monte Carlo simulations. Gamma-ray transmission was analyzed over an energy range of 0.276-1.332 MeV, and fast neutron attenuation was assessed at 4.5 MeV. The results showed that transmission factors decreased with increasing coating thickness, with the effect being more pronounced at lower photon energies. Among the investigated compositions, the Hf-based system exhibited the most favorable predicted attenuation response for both gamma rays and fast neutrons under the defined simulation conditions. Theoretical half-value layer calculations also showed good agreement with the simulation results. Overall, the findings indicate that high-entropy rare-earth oxide coatings may provide an additional radiation attenuation contribution when incorporated as layers in Inconel-718-based systems. However, since direct thermal-barrier properties such as thermal conductivity, thermal diffusivity, thermal cycling resistance, and thermal-stress behavior were not evaluated in the present work, the present study should be interpreted as a structural and radiation-transport assessment of TBC-related coating candidates rather than a direct demonstration of thermal-barrier performance.