Mixture behavior and microwave dielectric properties of (1  x)CaWO4xTiO2

https://doi.org/10.1016/j.jeurceramsoc.2006.11.035Get rights and content

Abstract

The microwave dielectric characteristics and mixture behavior of (1  x)CaWO4xTiO2 ceramics prepared with conventional solid-state route were studied using a network analyzer and X-ray power diffraction, respectively. The CaWO4 compound had good properties (low permittivity and high quality factor) for microwave applications, but it had a high negative temperature coefficient of resonant frequency (τf = −53). Hence, in order to tune the dielectric properties, (1  x)CaWO4xTiO2 were prepared for different values of x. X-ray powder diffraction and SEM analysis revealed that CaWO4 and TiO2 coexisted as a mixture. The mixture formation and dielectric properties could be explained by mixture rule. In particular, at x = 2.6, good microwave dielectric properties were obtained: Qf = 27,000, ɛr = 17.48, and τf = ∼0 ppm/°C.

Introduction

According to the development of high-frequency communication technology, microwave dielectric materials with stable temperature coefficient of resonant frequency (near zero) and lower dielectric loss (higher quality factor value) have been required. Searching for microwave dielectric materials with both stable temperature coefficient of resonant frequency and higher quality factor is constantly needed in ceramic material research.1 In our previous study, compounds with the general formula AWO4 (A = Mg, Mn, Zn, Ca, Sr, Ba) are found promising materials for microwave substrate application.2 These materials exhibit good microwave properties, high quality factor and low permittivity but with a high negative temperature coefficient resonant frequency around −50 ppm/°C. The most popular method of achieving stable temperature coefficient of resonant frequency is mixing materials, which have opposite value.3 In this way mixed materials form solid solution or mixture and show stable temperature coefficient of resonant frequency. The present investigation revealed that the τf of CaWO4 can be adjusted to zero with TiO2 addition.

Section snippets

Experimental

The used starting materials were CaCO3 (high purity chemicals, 99.99%), WO3 (high purity chemicals, 99.9%) and TiO2 (high purity chemicals, 99.9%). The CaWO4 powders were prepared using conventional mixed oxide method by calcining at 800 °C for 2 h. CaWO4 and TiO2 powders were mixed for varying composition according to the formula (1  x)CaWO4xTiO2 (x = 0.0, 0.1, 0.15, 0.2, 0.24, 0.25, 0.26, 0.3, 0.4, 0.5, 0.7, 0.9 and 1.0) and were ball-milled with ZrO2 balls for 24 h using ethanol. After drying

Result and discussion

Fig. 1 represents the X-ray diffraction (XRD) patterns for x = 0, 0.2, 0.3, 0.4, 0.5, 0.7, 0.9 and 1 in (1  x)CaWO4xTiO2. With increasing TiO2 content, the intensity of the reflections of CaWO4 phase decreased and those of TiO2 phase increased without peak shift. The XRD pattern data indicates that CaWO4 and TiO2 behave as mixture and not a solid solution and no second phase was found. Therefore, the dielectric properties of (1  x)CaWO4xTiO2 are proportional to their variation of the molar

Conclusion

The mixture behavior and microwave dielectric properties of CaWO4 with TiO2 system were investigated. The dielectric constant was increased with the molar addition of TiO2 into CaWO4 to form mixtures based on (1  x)CaWO4xTiO2. The analysis of the crystal structure by XRD indicated that no additional second phase was formed and (1  x)CaWO4xTiO2 exist as mixture in the entire range. The densities of mixture were over 97% of theoretical density and effects of porosity on dielectric properties

Acknowledgements

This research was supported by a grant from the Center for Advances Materials Processing (CAMP) of the 21st Century Frontier R&D Program funded by the Ministry of Commerce Industry and Energy (MOCIE), Republic of Korea.

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