Dielectric properties of (Mg
(1−x)Co
x)
4Ta
2O
9 (
x = 0.01 to 0.09) prepared by solid state reaction were investigated. The maximum properties of the (Mg
(1−x)Co
x)
4Ta
2O
9 (
x = 0.05) system were namely, an obtained ε
r value of 12.27, a Q×f value of 440,000 GHz, and a τ
f value of −59 ppm/°C sintered at 1325°C. The theoretical polarizability of (Mg
(1−x)Co
x)
4Ta
2O
9 increased with Co substitution,
x. (Mg
(1−x)Co
x)
4Ta
2O
9 with Mg
2+ substituted by and Co
2+ not only improved the microwave dielectric properties, but also decreased sintering temperature. From the calculation of the covalency of cation–oxygen bonds, it is found that the covalency of the Co–O bond is lower than that of the Mg–O bond and the difference in the covalency between these cation–oxygen bonds influences the temperature dependence of dielectric constant on the compounds. From our experiment, the best microwave dielectric property happens in (Mg
0.95Co
0.05)
4Ta
2O
9 sintered at 1325°C for 4 h, and it’s Q×
f is 440,000 GHz with τ
f = 59.5 ppm/°C.
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