High-entropy A₂B₂O₇-type oxide ceramics: A potential immobilising matrix for high-level radioactive waste

The sustainable development of civil nuclear energy requires the fabrication of the durable nuclear wasteforms, in particular for high-level radioactive waste, which involves the design of the composition and microstructure. Herein, we demonstrated that high-entropy ceramics (Eu_1-xGd_x)₂(Ti_0.2Zr_0.2Hf_0.2Nb_0.2Ce_0.2)₂O₇ are the potential candidate as immobilizing hosts for high-level radioactive waste. The static aqueous leaching test indicates that the normalized leaching rates for the simulated radionuclides Ce (LR_Ce) and Gd (LR_Gd) in as-prepared high-entropy ceramics are approximately 10^-6~10^-8 g·m^-2·d^-1 after 42 days testing, much lower than those reported values in doped-Gd₂Zr₂O₇ (10^-6~10^-3 g·m^-2·d^-1). The excellent chemical durability is mainly due to the synergistic effects of the compositional complexity and severe lattice distortion. Compared to their ternary oxides, the low oxygen vacancy concentration slows down the migration and diffusion of cations. Moreover, the lattice distortion increases the lattice potential energy, also inhibiting the migration of cations. This study provides a strategy for the development and application of high-entropy ceramics as the wasteforms.