Low-permittivity microwave dielectric ceramics are essential for high-frequency communication and radar systems, as they minimize signal delay and interference, thereby enabling compact and high-performance devices. In this study, LiAl_5−xNi_xO_8−0.5x (x = 0.1–0.5) ceramics were synthesized via a solid-state reaction method to investigate the effects of Ni²⁺ substitution on crystal structure, microstructure, and dielectric properties. X-ray diffraction and Rietveld refinement reveal a phase transition from the P4₃32 to the Fd$\stackrel{-}{3}$m spinel structure at x ≈ 0.3, accompanied by a systematic increase in the lattice parameter (7.909–7.975 Å), attributed to the larger ionic radius of Ni²⁺ compared to Al³⁺. SEM analysis confirms dense microstructures with relative densities exceeding 95% and grain size increases from less than 1 μm at x = 0.1 to approximately 2 μm at x = 0.5. Dielectric measurements show a decrease in permittivity (ε_r) from 8.24 to 7.77 and in quality factor (Q × f) from 34,605 GHz to 20,529 GHz with increasing Ni content, while the temperature coefficient of the resonant frequency (τ_f) shifts negatively from −44.8 to −69.1 ppm/°C. Impedance spectroscopy indicates increased conduction losses and reduced activation energy with higher Ni²⁺ concentrations.

Microwave dielectric ceramics are indispensable in modern communication technologies, playing a pivotal role in components such as filters, oscillators, and antennas. Among these materials, ZnAl₂O₄ ceramics have garnered attention for their excellent quality factor (Q × f) and low dielectric constant (ε_r). However, their high sintering temperature (~1650 °C) limits practical applications. This study investigates ZnAl_2-x(Zn_0.5Si_0.5)_xO₄ (ZAZS) (x = 0.1–0.9) ceramics, where [Zn_0.5Si_0.5]³⁺ substitutes Al³⁺, to reduce sintering temperature while maintaining high-performance microwave dielectric properties. ZAZS ceramics were synthesized via the solid-state reaction method and characterized for their structural, morphological, and dielectric properties. X-ray diffraction analysis confirmed the formation of a single-phase solid solution up to x = 0.8, with minor secondary phases appearing at x = 0.9. The substitution increased lattice parameters and enhanced material densification, as observed through SEM and relative density calculations. Microwave dielectric measurements showed that ZAZS ceramics achieved a maximum Q × f of 20,200 GHz and a τ_f value reduced to −62 ppm/°C at x = 0.8, while ε_r decreased from 7.90 to 6.98. Bond-valence calculations reveal that the reduction of the average Al/Zn/Si–O bond valence weakens octahedral rigidity, systematically tuning τ_f toward zero. These results demonstrate that ZAZS ceramics, with a reduced sintering temperature of 1400 °C, exhibit excellent potential for application in low-loss microwave devices.