In this paper, Ce2[Zr1−x(Cd1/3Sb2/3)x]3(MoO4)9 (CZ1−x(CS)xM, x = 0.01–0.1) were prepared via the conventional solid-state method. XRD and Rietveld refinement analyses confirmed the formation of a single-phase CZ1−x(CS)xM solid solution with a space group of R-3c(167). The sintering behavior of the samples were investigated using SEM and relative density, which showed that optimal densification for CZ0.98(CS)0.02M ceramics were achieved at 675 °C with an average grain size of 1.70 μm. The P-V-L theory revealed the significant influence of the Zr(Cd/Sb)-O bond on the dielectric properties of CZ1−x(CS)xM ceramics. Furthermore, far-IR reflectance spectra indicated that the measured dielectric loss value (1.04 × 10−4) is in line with the calculated value (1.60 × 10−4), suggesting a substantial impact of phonon oscillation absorption on the dielectric properties. Notably, CZ0.98(CS)0.02M ceramics demonstrated superior performance at 675 °C, with εr = 10.44, Q × f = 93,152 GHz (at 12.96 GHz), and τf = −17.73 ppm/°C.
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