Preparation, structures, thermal properties and sintering behaviors of B₂O₃-SiO₂-ZnO-BaO-Al₂O₃ glass

Abstract

B₂O₃-SiO₂-ZnO-BaO-Al₂O₃ glass with different Al₂O₃ contents (1mol%, 3mol%, 5mol%, and 7mol%) was prepared, and it was intended to be used as lead-free and low-melting glass sealants for solid oxide fuel cells. The effects of Al₂O₃ content on the structures, thermal properties, and sintering behaviors of the B₂O₃-SiO₂-ZnO-BaO-Al₂O₃ glass were investigated in detail. The Al₂O₃ content largely influenced the structures and thermal properties of the glass. When the Al₂O₃ content 5mol%, the transition temperature of the glass decreased with the Al₂O₃ content, while the crystallization temperature increased with the Al₂O₃ content. However, higher Al₂O₃ content degraded the stability of the glass. The B₂O₃-SiO₂-ZnO-BaO-Al₂O₃ glass with 5 mol% Al₂O₃ content exhibits the optimal sintering densification characteristics and can be used as glass sealants for solid oxide fuel cells.

Keywords

B₂O₃-SiO₂-ZnO-BaO-Al₂O₃ glass / thermal properties / sintering behavior / densification / crystallization

References

[1] Hwang GH, Jeon HJ, Kim YS. Physical Properties of Barrier Ribs of Plasma Display Panels: I, Formation of Pores during Sintering of Lead Borosilicate Glass Frits[J]. J. Am. Ceram. Soc., 2002, 85: 2956-2960.

[2] Lim ES, Kim BS, Lee JH, et al. Effect of BaO Content on the Sintering and Physical Properties of BaO-B₂O₃-SiO₂ Glasses[J]. J. Non-Cryst. Solids, 2006, 352: 821-826.

[3] Buchanan RC, Zuegel MA. Eletrical Properties of Glasses in the System PbO-Al₂O₃-B₂O₃-SiO₂[J]. J. Am. Ceram. Soc., 1968, 51: 28-32.

[4] Singh D, Singh K, Singh G, et al. Optical and Structural Properties of ZnO-PbO-B₂O₃ and ZnO-PbO-B₂O₃-SiO₂ Glasses[J]. J. Phys.: Cond. Matt., 2008, 20: 075228-6.

[5] Adachi K, Kuno H. Decomposition of Ruthenium Oxides in Lead Borosilicate Glass[J]. J. Am. Ceram. Soc., 1997, 80: 1055-1064.

[6] Monteiro RCC, Lopes AAS, Lima M, et al. Sintering, Crystallization, and Dielectric Behavior of Barium zinc Borosilicate Glasses-effect of Barium Oxide Substitution for Zinc Oxide[J]. J. Am. Ceram. Soc., 2012, 95: 3144-3150.

[7] Shih PY, Chin TS. Preparation of Lead-free Phosphate Glasses with Low Tg and Excellent Chemical Durability[J]. J. Mater. Sci. Lett., 2001, 20: 1811-1813.

[8] Hsu JH, Kim CW, Brow RK, et al. An Alkali-free Barium Borosilicate Viscous Sealing Glass for Solid Oxide Fuel Cells[J]. J. Power Sources, 2014, 270: 14-20.

[9] Wang SF, Wang YR, Hsu YF, et al. Effect of Additives on the Thermal Properties and Sealing Characteristic of BaO-Al₂O₃-B₂O₃-SiO₂ Glass-Ceramic for Solid Oxide Fuel Cell Application[J]. Inter. J. Hydrogen Energy, 2009, 34: 8235-8244.

[10] Steele BCH, Heinzel A. Materials for Fuel-cell Technologies[J]. Nature, 2001, 414: 345-352.

[11] Pascual MJ, Guillet A, Durán A. Optimization of Glass-ceramic Sealant Compositions in the System MgO-BaO-SiO₂ for Solid Oxide Fuel Cells (SOFC)[J]. J. Power Sources, 2007, 69: 40-46.

[12] Hassmann K, Rippel R. A New Approach to Fuel Cell Investment Strategy[J]. J. Power Sources, 1998, 71: 75-79.

[13] Lopes AAS, Soares RS, Lima MMA, et al. Glass Transition and Crystallization Kinetics of a Barium Borosilicate Glass by a Nonisothermal Method[J]. J. Appl. Phys., 2014, 115: 043516-9.

[14] Lim ES, Kim BS, Lee JH, et al. Characterization of the Low Temperature Firing BaO-B₂O₃-SiO₂ Glass: The Effect of BaO Content[J]. J. Eur. Ceram. Soc., 2007, 27: 825-829.

[15] Ramkumar J, Chandramouleeswaran S, Sudarsan V, et al. Barium Borosilicate Glass as a Matrix for the Uptake of Dyes[J]. J. Hazard. Mater., 2009, 172: 457-464.

[16] Hu AM, Li M, Dali DLM, et al. Crystallization and Properties of a Spodumene-willemite Glass Ceramic[J]. Thermochim. Acta, 2005, 437: 110-113.

[17] Zhou L, Lin H, Chen W, et al. IR and Raman Investigation on the Structure of (100-x) B₂O_3–x(0.5BaO-0.5ZnO) Glasses[J]. J. Phys. Chem. Solids, 2008, 69: 2499-2502.

[18] Sun T, Xiao H, Guo W, et al. Effect of Al₂O₃ Content on BaO-Al₂O₃-B₂O₃-SiO₂ Glass Sealant for Solid Oxide Fuel Cell[J]. Ceram. Inter., 2010, 36: 821-826.

[19] Efimov AM. Quantitative IR Spectroscopy: Applications to Studying Glass Structure and Properties[J]. J. Non-Cryst. Solids, 1996, 203: 1-11.

[20] Richet P, Atake T, Yamashita I. Boroxol Rings in SiO₂-B₂O₃ Glasses: Influence on Low-temperature Thermal Properties[J]. J. Non-Cryst. Solids, 2006, 352: 3854-3858.

[21] Cheng Y, Xiao H, Guo W, et al. Structure and Crystallization Kinetics of PbO-B₂O₃ Glasses[J]. Ceram. Inter., 2007, 33: 1341-1347.

[22] Bobkova NM, Khotko SA. Structure of Zinc-borate Low-melting Glasses Derived from IR Spectroscopy Data[J]. J. Appl. Spectroscopy, 2005, 72: 853-857.

[23] Arora M, Baccaro S, Sharma G, et al. Radiation Effects on PbO-Al₂O₃-B₂O₃-SiO₂ Glasses by FTIR Spectroscopy[J]. Nucl. Instru. Methods Phys. Res., 2009, 267: 817-820.

[24] Kamitsos EI, Patsis AP, Karakassides MA, et al. Infrared Reflectance Spectra of Lithium Borate Glasses[J]. J. Non-Cryst. Solids, 1990, 126: 52-67.

[25] Kamitsos EI, Patsis AP, Chryssikos GD. Infrared Reflectance investigation of alkali diborate glasses[J]. J. Non-Cryst. Solids, 1993, 152: 246-257.

[26] Cheng Y, Xiao H, Guo W, et al. Structure and Crystallization Kinetics of Bi₂O₃-B₂O₃ Glasses[J]. Thermochim. Acta, 2006, 444: 173-178.

[27] Khalkhali Z, Hamnabard Z, Qazvini SSA, et al. Preparation, Phase Formation and Photoluminescence Properties of ZnO-SiO₂-B₂O₃ Glasses with Different ZnO/B₂O₃ Ratios[J]. Opt. Mater., 2012, 34: 850-855.

[28] Hrubý A. Evaluation of Glass-forming Tendency by Means of DTA[J]. Czech. J. Phys. B, 1972, 22: 1187-1193.

[29] Mahadevan S, Giridhar A, Singh AK. Calorimetric Measurements on As-Sb-Se Glasses[J]. J. Non-Cryst. Solids, 1986, 88: 11-34.

[30] Demirkesen E, Maytalman E. Effect of Al₂O₃ Additions on the Crystallization Behaviour and Bending Strength of a Li₂O-ZnO-SiO₂ Glass-ceramic[J]. Ceram. Inter., 2001, 27: 99-104.

[31] Fairweather MJ, Topping JA, Murthy MK. Effect of Al₂O₃ on a Complex Li₂O-ZnO-SiO₂ Glass-ceramic[J]. J. Am. Ceram. Soc., 1975, 58: 260-261.

[32] Qazvini SSA, Hamnabard Z, Khalkhali Z, et al. Photoluminescence and Microstructural Properties of SiO₂-ZnO-B₂O₃ System Containing TiO₂ and V₂O₅[J]. Ceram. Inter., 2012, 38: 1663-1670.

[33] Hu Y, Tsai HT. The Effect of BaO on the Crystallization Behaviour of a Cordierite-type Glass[J]. Mater. Chem. Phys., 1998, 52: 184-188.

[34] Gödeke D, Dahlmann U. Study on the Crystallization Behaviour and Thermal Stability of Glass-ceramics Used as Solid Oxide Fuel Cellsealing Materials[J]. J. Power Sources, 2011, 196: 9046-9050.

[35] Lara C, Pascual MJ, Prado MO, et al. Sintering of Glasses in the System RO-Al₂O₃-BaO-SiO₂ (R=Ca, Mg, Zn) Studied by Hot-stage Microscopy[J]. Solid State Ionics, 2004, 170: 201-208.

[36] He F, Wang J, Deng D. Research of the Bi₂O₃ Content Effect on the Bi₂O₃-ZnO-B₂O₃ System Glass[C]. The National Glass Science and Technology Annual Meeting, 2009

[37] Sohn SB, Choi SY, Kim GH, et al. Stable Sealing Glass for Planar Solid Oxide Fuel Cell[J]. J. Non-Cryst. Solids, 2002, 297: 103-112.