Na₂O/Li₂O Ratio Dependency on the Thermal, Mechanical, Dielectric Properties and Chemical Stabilities of Li₂O-Al₂O₃-SiO₂ Glass

Abstract

Li₂O-Al₂O₃-SiO₂ based glasses were investigated as potential protection glass for electronic devices due to their excellent mechanical properties, such as high hardness, toughness, and scratch resistance. In this paper, Li₂O-Na₂O-Al₂O₃-SiO₂ glass with different Li₂O/Na₂O ratio components were prepared by melt-quenching method, and the effects of Na₂O/Li₂O ratio on the glass densities, structure, thermal, mechanical properties, and chemical stabilities were studied. The experimental results indicate that the glass transition temperature increases with the increases in Na₂O/Li₂O ratios, due to larger ion radius. While the thermal expansion coefficient slightly decreases from 11.4 × 10⁻⁶ to 11.09 × 10⁻⁶/°C. The elastic modulus increases from 57 to 72 GPa. The bending strength reaches maximum 80.90 MPa when the Na₂O/Li₂O ratio is 1.7, then decreases as the ratio further increases. In addition, the Vicker’s hardness gets to 7.37 GPa with largest Na₂O/Li₂O ratio. Moreover, the dielectric loss and dielectric constant increases as the ratio increases. The Raman structure analysis shows the Q₄ [Si-O-Si] decreases as Na₂O/Li₂O ratio increases, which is responsible for the characteristic properties change. Moreover, the glass shows lowest mass loss in 10vol% HF solutions when the ratio is 1.4, while 1.7 in 5wt% NaOH solution.

Keywords

glass composition / dielectric constant / coefficient of thermal expansion / elastic modulus

References

[1] Ahmina W, El Moudane M. Chemical Durability, Electrical and Dielectric Properties of the Ternary System (50-x)K₂O_1−xMnO-50P₂O= Phosphate Glasses[J]. Materials Today: Proceedings, 2019, 13: 466-473.

[2] Aliyah LH, Izzat BM et al. Effect of Mechanical Properties on Sintered Lithium Aluminosilicate Glass Ceramic and Its Thermal Shock Resistance Properties[C]. In: 3rd International Postgraduate Conference on Materials, Minerals & Polymer, 2020, 2267: 020047-1-8

[3] Chen R, Jia W, et al. Improvement of the Alkali Corrosion Resistance and Mechanical Properties of Corundum Castables by Coating of Li₂O-Al₂O₃-SiO₂ Glaze[J]. Journal of the Australian Ceramic Society, 2019, 55: 703-710.

[4] Dechandt ICJ, Soares P, Pascual MJ. Sinterability and Mechanical Properties of Glass-ceramics in the System SiO₂-Al₂O₃-MgO/ZnO[J]. Journal of the European Ceramic Society, 2020, 40: 6 002-6 013.

[5] Donald IW, Metcalfe BL, Fong SK. The Influence of Fe₂O₃ and B₂O₃ Additions on the Thermal Properties, Crystallization Kinetics and Durability of a Sodium Aluminum Phosphate Glass[J]. Journal of Non-Crystalline Solids, 2006, 352: 2 993-3 001.

[6] Doweidar H. Density of CaO-Al₂O₃-SiO₂ Glasses with (CaO/Al₂O₃) ⩾ 1: The Hidden Factors[J]. Journal of Non-Crystalline Solids, 2017, 471: 344-348.

[7] Gong L, Wang Y, Cheng X. Porous Mullite Ceramics with Low Thermal Conductivity Prepared by Foaming and Starch Consolidation[J]. Journal of Porous Materials, 2013, 21: 15-21.

[8] Meng J, Peng J. Preparation and Properties of Endothermic Functional Ceramics with Iron Tailings as Raw Materials[J]. Materials Research Express, 2020, 7: 055 501-055 509.

[9] Shi J, He F, Xie J. Exploring the Influences of Li₂O/SiO₂ Ratio on Li₂O-Al₂O₃-SiO₂-B₂O₃-BaO Glass-ceramic Bonds for Vitrified cBN Abrasives[J]. Ceramics International, 2019, 45: 15 358-15 365.

[10] Habasaki J, Ngai KL. The Mixed Alkali Effect in Ionically Conducting Glasses Revisited: A Study by Molecular Dynamics Simulation[J]. Physical Chemistry Chemical Physics, 2007, 9: 4 673-4 689.

[11] Xingzhong G, Lingjie Z, Hui Y. Effects of Li Replacement on the Nucleation, Crystallization and Microstructure of Li₂O-Al₂O₃-SiO₂ Glass[J]. Journal of Non-Crystalline Solids, 2008, 354: 4 031-4 036.

[12] Vegiri A, Varsamis CPE, Kamitsos EI. Molecular Dynamics Investigation of Mixed-alkali Borate Glasses: Short-range Order Structure and Alkali-ion Environments[J]. Physical Review B, 2009, 80: 1-12.

[13] Zhao F, Nan X, Fu Q. Mechanical Behavior of the Joints between Carbon/Carbon Composites and Li₂O-Al₂O₃-SiO₂ Glass Ceramics with YAS Interlayer at High Temperature[J]. Materials Science and Engineering: A, 2020, 772: 138 550-138 560.

[14] Zhang XH, Yue YL, Wu HT. Effects of Compositional Variation on the Structure and Properties of Aluminoborosilicate Glasses[J]. Key Engineering Materials, 2013, 538: 238-241.

[15] Wang WW, Yue YL, Zhang HT. Effect of Magnesium Additive on Structure and Properties of Al₂O₃-B₂O₃-SiO₂ Glass System[J]. Materials Technology, 2013, 28: 370-374.

[16] Vitucci G, Mishuris G. Analysis of Residual Stresses in Thermoelastic Multilayer Cylinders[J]. Journal of the European Ceramic Society, 2016, 36: 2 411-2 417.

[17] Tarafder A, Singh SP, Karmakar B. Effects of TiO₂-SiO₂ Fillers on Thermal and Dielectric Properties of Bismuth Glass Microcomposite Dielectrics for Plasma Display Panel[J]. Journal of Materials Science: Materials in Electronics, 2010, 22: 515-522.

[18] Smedskjaer MM, Jensen M, Yue Y. Effect of Thermal History and Chemical Composition on Hardness of Silicate Glasses[J]. Journal of Non-Crystalline Solids, 2010, 356: 893-897.

[19] Hussain I, Barimah EK. Mechanical and Optical Properties of ZrO2 Doped Silicate Glass Ceramics[J]. Silicon, 2020, 13: 877-883.

[20] Kasuga T, Kimata T, Obata A. Preparation of a Calcium Titanium Phosphate Glass-Ceramic with Improved Chemical Durability[J]. Journal of the American Ceramic Society, 2009, 92: 1 709-1 712.

[21] Lang Y, Wang CA. Al₂O₃-fiber-reinforced Porous YSZ Ceramics with High Mechanical Strength[J]. Ceramics International, 2014, 40: 10 329-10 335.

[22] Li H, Yin Z, Deng L. Effect of SiO₂/Al₂O₃ Ratio on the Structure and Electrical Properties of MgO-Al₂O₃-SiO₂ Glass-ceramics Doped with TiO₂[J]. Materials Chemistry and Physics, 2020, 256: 123 653.

[23] Li M, Li Y, Ouyang D. Effects of Alumina Bubble Addition on the Properties of Mullite Castables[J]. Journal of Alloys and Compounds, 2018, 735: 327-337.

[24] Liu J, Li Y, et al. Effects of Pore Structure on Thermal Conductivity and Strength of Alumina Porous Ceramics Using Carbon Black as Pore-forming Agent[J]. Ceramics International, 2016, 42: 8221-8228.

[25] Lutpi HA, Mohamad H. Effect of Isothermal Treatment on the Structural, Microstructure, and Physio-mechanical Properties of Li₂O-Al₂O₃-SiO₂ Glass-ceramic[J]. Journal of the Australian Ceramic Society 2021. https://doi.org/10.1007/s41779-021-00662-6

[26] Orlova LA, Chainikova AS, Alekseeva LA. Recent Advances in Radio Transparent Glass-Ceramic Materials Based on High-Temperature Aluminosilicate Systems[J]. Russian Journal of Inorganic Chemistry, 2015, 60: 1 692-1 707.

[27] Qi H, Fan Y, Xing W. Effect of TiO₂ Doping on the Characteristics of Macroporous Al₂O₃/TiO₂ Membrane Supports[J]. Journal of the European Ceramic Society, 2010, 30: 1 317-1 325.

[28] Ohashi KTM. Mixed-Alkali Effect on Rayleigh Scattering in K₂O-Na₂O-MgO-SiO₂ glass[J]. Journal of the American Ceramic Society, 2010, 83: 660-662.

[29] Honnavar GV, Ramesh KP, Bhat SV. Role of Crystal Field in Mixed Alkali Metal Effect: Electron Paramagnetic Resonance Study of Mixed Alkali Metal Oxyfluoro Vanadate Glasses[J]. The Journal of Chemical Physics, 2014, 118: 573-578.

[30] Rodrigues A, Fearn S, Vilarigues M. Mixed Reactions: Glass durability and the Mixed-alkali Effect[J]. Journal of the American Ceramic Society, 2019, 102: 7 278-7 287.

[31] Kojima S. Mixed-Alkali Effect in Borate Glasses: Thermal, Elastic, and Vibrational Properties[J]. Solids, 2020, 1: 16-30.

[32] Lodesani F, Menziani MC, Hijiya H. Structural Origins of the Mixed Alkali Effect in Alkali Aluminosilicate Glasses: Molecular Dynamics Study and its Assessment[J]. Scientific Reports, 2020, 10: 2 906-2 918.

[33] Onodera Y, Takimoto Y, Hijiya H. Origin of the Mixed Alkali Effect in silicate Glass[J]. NPG Asia Materials, 2019, 11: 75-86.

[34] Wilkinson CJ, Potter AR. Topological Origins of the Mixed Alkali Effect in Glass[J]. Journal Of Physical Chemistry B, 2019, 123: 7 482-7 489.

[35] Soares VO, Rodrigues AM. Improvements on Sintering and Thermal Expansion of Lithium Aluminum Silicate Glass-ceramics[J]. Ceramics International, 2020, 46: 17 430-17 436.

[36] Scannell G, Huang L, Rouxel T. Elastic Properties and Indentation Cracking Behavior of Na₂O-TiO₂-SiO₂ Glasses[J]. Journal of Non-Crystalline Solids, 2015, 429: 129-142.

[37] Ohashi K. Mixed Alkali Effect on Rayleigh Scattering in K₂O-Na₂O-MgO-SiO₂ Glasses[J]. Journal of the American Ceramic Society, 2000, 83: 660-662.

[38] Seidel S, Dittmer M, Holand W. High-strength, Translucent Glass-ceramics in the System MgO-ZnO-Al₂O₃-SiO₂-ZrO₂[J]. Journal of the European Ceramic Society, 2017, 37: 2 685-2 694.

[39] Mukherjee DP, Das SK. The influence of Content on the Properties of Glass Ceramics: Crystallization, Microstructure and Hardness[J]. Ceramics International, 2014, 40: 4 127-4 134.

[40] Shin H, Lee S-W, Jung HS. Sintering and Dielectric Properties of Li₂O-B₂O₃-Al₂O₃-SiO₂ Glass-Added (Ca_0.7Sr_0.3O)_1.03(Ti_0.1Z_0.9)O₂ for Copper Electrode[J]. International Journal of Applied Ceramic Technology, 2013, 10: 716-722.

[41] Raju GN, Ramesh NC. Spectroscopic and Dielectric Properties of Titanium Doped MgO-Al₂O₃-B₂O₃ Glass System[C]. IOP Conference Series: Materials Science and Engineering, 2009, 2: 012 031-012 035.

[42] Mansour E. Mixed Alkali Effect in Quaternary K₂O-Li₂O-BaO-B₂O₃ Glasses Containing V₂O₅[J]. Physical B: Condensed Matter, 2005, 362: 88-94.

[43] Le Losq C, Neuville DR, Florian P. The Role of Al³⁺ on Rheology and Structural Changes in Sodium Silicate and Aluminosilicate Glasses and Melts[J]. Geochimica et Cosmochimica Acta, 2014, 126: 495-517.

[44] Glatz P, Comte M. Different Roles of Phosphorus in the Nucleation of Lithium Aluminosilicate Glasses[J]. Journal of Non-Crystalline Solids, 2018, 493: 48-56.

[45] Brooker MH. Assessment of Correction Procedures for Reduction of Raman Spectra[J]. Journal of Raman Spectroscopy, 1988, 19: 71-78.