Synthesis, crystallization behavior, microstructure and mechanical properties of oxynitride glass-ceramics with fluorine addition

Abstract Y–Si–Al–O–N–F oxynitride glasses were prepared by melting batches at 1500–1700 °C for 2 h under N2 atmosphere in a Si–Mo-heated resistance furnace. The appropriate heat treatment temperatures were selected according to the information provided by the differential scanning calorimeter (DSC) measurement. X-ray diffraction (XRD) and scanning electron microscope (SEM) were used to study the crystallization behavior of the glass-ceramics. DSC analysis demonstrated that an increase in fluorine content lowers the crystallization temperature of the oxynitride glass at constant N content. XRD and SEM analysis demonstrated that, as the nitrogen content is 6 or 12 equiv. %, Y2Si2O7 began to appear in the base glass first, which reduces the amounts of Y and Si available to form mullite; as the nitrogen content increases to 18 equiv. %, Si3Al6O12N2 and mullite begins to appear first; at 24 equiv.% N, the only crystallization phase is mullite, Y, N and F remain in the residual glassy phase of the glass-ceramic. An increase in nitrogen content favors the formation of Si3Al6O12N2 or mullite (Al6Si2O13) rather than Y2Si2O7, suggesting that which phase may be able to accommodate N into its crystal structure. In terms of mechanical properties, micro-hardness is more sensitive to changes in the nitrogen content of the residual glass phase than the bending strength which is related to the amounts of crystallized phases, phase morphology and crystal size.

[1]  Wen-ru Sun,et al.  The effect of GPS parameters on mechanical properties of Y—α-SiAlON ceramics , 1997 .

[2]  Xiuying Li,et al.  Crystallization and microstructures of Y-Si-Al-O-N glass-ceramics containing main crystal phase Y3Al5O12 , 2011 .

[3]  D. Wood,et al.  Influence of Fluorine Content in Apatite–Mullite Glass‐Ceramics , 2004 .

[4]  S. Hampshire,et al.  Effects of nitrogen and fluorine on crystallisation of Ca–Si–Al–O–N–F glasses , 2012 .

[5]  D. Thompson,et al.  Heat treatment of wollastonite-type Y–Si–Al–O–N glasses , 1997 .

[6]  M. I. Alayo,et al.  Study of the mechanical and structural properties of silicon oxynitride films for optical applications , 2006 .

[7]  I. Kityk,et al.  SiON films deposited on Si(111) substrates—new promising materials for nonlinear optics , 1999 .

[8]  Lu An-xian,et al.  Effects of heat treatment schedule on crystallization behaviors of Mg-Y-Al-Si-O-N glasses , 2009 .

[9]  M. Graça,et al.  Dielectric analysis of tungsten–phosphoniobate 20A2O–30WO3 –10Nb2O5 –40P2O5 (A = Li, Na) glass–ceramics , 2011 .

[10]  M. Ghaffari,et al.  Sintering behavior and mechanical properties of mica-diopside glass–ceramic composites reinforced by nano and micro-sized zirconia particles , 2012 .

[11]  D. Rao,et al.  Influence of molybdenum ions on spectroscopic and dielectric properties of ZnF2–Bi2O3–P2O5 glass ceramics , 2012 .

[12]  K. Jack.  Sialons and related nitrogen ceramics , 1976 .

[13]  P. Miranzo,et al.  Sintering behaviour and properties of YAlSiO and YAlSiON glass-ceramics , 2011 .

[14]  S. Hampshire.  Oxynitride glasses, their properties and crystallisation – a review , 2003 .

[15]  V. Kumar,et al.  Piezoelectric and elastic properties of ZnF2–PbO–TeO2: TiO2 glass ceramics , 2012 .

[16]  Tanguy Rouxel,et al.  Yttrium oxynitride glasses: Properties and potential for crystallisation to glass-ceramics , 1994 .

[17]  C. Ahn,et al.  Characterization and Crystallization of Y‐Si‐Al‐O‐N Glass , 1982 .

[18]  T. Rouxel,et al.  Yttrium sialon glasses: Nucleation and crystallization of Y35Si45Al20O83N17 , 1997 .

[19]  S. Sakka.  Structure, properties and application of oxynitride glasses , 1995 .

[20]  C. Brinker,et al.  Oxynitride glasses prepared from gels and melts , 1983 .

[21]  S. Hampshire,et al.  Classical and Differential Thermal Analysis Studies of the Glass‐Ceramic Transformation in a YSiAlON Glass , 2005 .

[22]  T. Rouxel,et al.  Crystallization and properties of a Si-Y-Al-O-N glass ceramic , 1993 .