Surface and bulk crystallization of Ba1-xSrxZn2Si2O7 from glasses in the system BaO/SrO/ZnO/SiO2 doped with Nb2O5 or Ta2O5

Stoichiometric 0.5 BaO·0.5 SrO·2 ZnO·2 SiO2 glass was doped with 5 mol% Nb2O5 or Ta2O5. The effect of these additives on the crystallization behavior was studied using thermal analyses, X-ray diffraction, as well as scanning electron microscopy including elemental analyses. The addition of Nb2O5 or Ta2O5 significantly increases the glass stability enabling the preparation of crystal-free BaO·SrO·ZnO·SiO2 glasses with almost stoichiometric composition. Besides the desired main crystal phase Ba1-xSrxZn2Si2O7, also alkaline earth tantalates and niobates as well as Zn2SiO4 are observed. The Nb-containing glass shows solely surface crystallization, whereas in the Ta-containing glass, additionally numerous barium tantalate crystals precipitate in the bulk acting as seeds for the nucleation of Ba1-xSrxZn2Si2O7. If the surface crystallized layer of Ba1-xSrxZn2Si2O7 approaches such a barium tantalate crystal or gets close to it, then the crystallization of Ba1-xSrxZn2Si2O7 is initiated. It is supposed that these nucleation processes are notably facilitated by the stresses present in these glass-ceramics.