Effect of Co2+ substitution on the phase evolution, densification behavior, and microwave dielectric properties of Zn1.8-xCoxSiO3.8 ceramics
摘要
Low-permittivity microwave dielectric ceramics with nominal compositions Zn1.8-xCoxSiO3.8 (x = 0–0.12) were synthesized by a solid-state reaction route. The influence of Co2+ substitution on phase evolution, lattice structure, densification behavior, and microwave dielectric performance was systematically evaluated. X-ray diffraction coupled with Rietveld refinement verifies that all specimens in the investigated range preserve a single-phase Zn2SiO4 (willemite) solid-solution structure, with no detectable secondary phases. Microstructural observations indicate that a small Co2+ addition facilitates mass transport along grain boundaries and assists pore removal, thereby enhancing densification at relatively low sintering temperatures. The composition with x = 0.04 exhibited the best overall performance, with a bulk density of 4.0893 g/cm3 and a relative density of 96.17%. At a resonant frequency of 13.121 GHz, the dielectric properties were εr = 6.55, Q × f = 62,559.8 GHz, and τf = − 45.2 ppm/℃. Meanwhile, the optimum sintering temperature was reduced to 1275 ℃. In contrast, further increasing Co content (x ≥ 0.06) introduces more grain-boundary imperfections and residual porosity, which compromises densification, decreases Q × f, and weakens the improvement in τf. Benefiting from the combination of low permittivity and high-quality factor, the developed Zn2SiO4-based ceramics show potential for high-frequency communication components. These results demonstrate that Co2+ doping offers an effective pathway to achieve low-temperature densification while coordinating dielectric performance in willemite-type low-loss microwave ceramics.