When Pr and Y ions are added to M-type strontium ferrite, a portion of the ions will enter the main phase lattice, while the excess ions will aggregate at the grain boundaries to form a secondary phase. The occupancy of rare earth ions in the main phase lattice and the formation of secondary phases are two key factors affecting the material's absorbing properties. The difference in ultimate solid solubility between rare earth ions Pr and Y in M-type strontium ferrite is significant, and they also form different secondary phases at grain boundaries. Consequently, the synthesized SrFe12-2xPrxYxO19 (0 < x ≤ 1.5) demonstrates its potential as a microwave absorbing material across a wide range of substitutions. Moreover, the performance changes have their own characteristics at different substitution levels. XRD results show that the samples include pure M phase and the coexistence of M phase and heterogeneous phases, with the heterogeneous phases being perovskite-type and garnet-type. SEM and EDS results indicate that Pr and Y co-substitution can refine grain size and reduce oxygen content. XPS results suggest that the valence change of Pr ions leads to the generation of Fe2+ ions and oxygen vacancies (Od). PPMS results reveal that saturation magnetization and coercivity are mainly affected by anisotropy field and particle size. Co-substitution of Pr and Y increases the dielectric and magnetic losses of the M phase, and the generated heterogeneous phases also enhance the dielectric and magnetic losses through interface polarization and magnetic exchange coupling effects, both cooperatively improving the wave-absorbing performance, with the minimum reflection loss (RLmin) reaching −51.57 dB (x = 0.1, d1 = 4.0 mm, EAB = 2.57 GHz).
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