High crystallization, low-dielectric-loss Li
2O–
xMgO–ZnO–B
2O
3–SiO
2 (
x = 30, 35, 40, 45 and 50 wt.%) (LMZBS) glass–ceramics were prepared with different MgO contents using the solid-state method in this study. The effects of the MgO content on the microstructures, flexural strength and microwave dielectric properties of LMZBS were investigated. X-ray diffractometer results, for samples sintered at 920°C, for 30 wt.% ≤
x ≤ 35 wt.%, showed that the main phase was Mg
2B
2O
5 and the secondary phase was Li
2ZnSiO
4. But a new Mg
3B
2O
6 phase appeared when the MgO content exceeded 35 wt.%, becoming the main phase at
x = 50 wt.%. Scanning electron microscopy showed that the average grain size decreased with increases in MgO and that a compact, homogeneous microstructure could be obtained at
x = 40 wt.%. The
Q×
f value (product of qualify factor and resonant frequency) increased at first due to increases in the theoretical
Q (quality factor) value and relative density, and then decreased due to a decrease in the average grain size and the appearance of large amounts of the liquid phase. Finally, the Li
2O–
xMgO–ZnO–B
2O
3–SiO
2 glass-ceramics with 40 wt.% MgO exhibited excellent microwave properties and mechanical properties in terms of dielectric constants (ε
r = 6.66),
Q×
f = 54600 GHz, temperature coefficient of resonant frequency (τ
f = −35 ppm/°C) and flexural strength (σ = 160 MPa) after the samples were sintered at 920°C for 2 h in air, indicating their suitability as low-temperature co-fired ceramics.
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