Preprint Article Version 1 Preserved in Portico This version is not peer-reviewed

Crystallization Behavior of Na2O-GeO2-P2O5 Glass System: (Micro)Structural, Electrical, and Dielectric Study

Version 1 : Received: 7 December 2023 / Approved: 7 December 2023 / Online: 7 December 2023 (11:01:37 CET)

A peer-reviewed article of this Preprint also exists.

Marijan, S.; Razum, M.; Sklepić Kerhač, K.; Mošner, P.; Koudelka, L.; Pisk, J.; Moguš-Milanković, A.; Skoko, Ž.; Pavić, L. The Crystallization Behavior of a Na2O-GeO2-P2O5 Glass System: A (Micro)Structural, Electrical, and Dielectric Study. Materials 2024, 17, 306. Marijan, S.; Razum, M.; Sklepić Kerhač, K.; Mošner, P.; Koudelka, L.; Pisk, J.; Moguš-Milanković, A.; Skoko, Ž.; Pavić, L. The Crystallization Behavior of a Na2O-GeO2-P2O5 Glass System: A (Micro)Structural, Electrical, and Dielectric Study. Materials 2024, 17, 306.

Abstract

Sodium-phosphate-based glass-ceramics (GCs) are promising materials for a wide range of applications, including solid-state sodium-ion batteries, microelectronic packaging substrates, and humidity sensors. This study investigates the impact of 24-hour heat-treatments at varying temperatures on Na-Ge-P glass, with a focus on (micro)structural, electrical, and dielectric properties of prepared GCs. Various techniques such as powder X-ray diffraction (PXRD), infrared spectroscopy-attenuated total reflection (IR-ATR), and scanning electron microscopy-energy dispersive spectroscopy (SEM-EDS) are employed. With the elevation of heat-treatment temperature, crystallinity progressively rises; at 450 °C, the microstructure retains amorphous traits featuring nanometric grains, whereas at 550 °C, heat-treatment results in fully crystallized structures characterized by square-shaped micron-scale grains of NaPO3. The insight into the evaluation of electrical and dielectric properties is provided by Solid-State Impedance Spectroscopy (SS-IS), revealing a strong correlation with the conditions of controlled crystallization and observed (micro)structure. The glass-ceramic heat-treated at 450 °C achieves the highest DC conductivity of 2.30×10–8 Ω–1 cm–1 at 393 K. As the heat-treatment temperature rises, the crystallization of the NaPO3 phase depletes the glass matrix of mobile Na+ ions, resulting in a reduction in DC conductivity. Dielectric parameters also decrease with rising heat-treatment temperature, with the glass-ceramic heat-treated at 550 °C displaying the lowest permittivity of 19.37 and the dielectric loss of 0.008. This research uncovers the intricate relationship between heat-treatment conditions and material properties, emphasizing that controlled crystallization allows for precise modifications to microstructure and phase composition within remaining glassy phase, ultimately facilitating fine-tuning of material properties.

Keywords

phosphate glasses; phosphate glass-ceramics; controlled crystallization; (micro)structure-property relationship; IR-ATR; PXRD; SEM-EDS; Solid-State Impedance Spectroscopy (SS-IS)

Subject

Chemistry and Materials Science, Ceramics and Composites

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