Mold material and dimension effects on the microstructural gradient in a glass-ceramic

Abstract

Microstructural gradients can significantly affect the properties of glass-ceramics (GCs). Such spatial variations in glass-ceramic (GC) microstructure may result from a non-uniform cooling rate when the glass-forming liquid is cast into a mold. This study investigates the material and mold size influence on the cooling process, leading to a non-uniform distribution of crystalline nuclei in the parent glass. We used a high-nucleation rate, non-stoichiometric, lithium metasilicate GC as a model. Initially, the glass-forming liquid was cooled in cylindrical molds with diameters of 7 and 14 mm, made from copper and 304 stainless steel – materials with distinct thermal diffusivities. Simulated thermography, validated by thermocouple data, showed contrasting cooling profiles across the samples. Our key findings are: i) cooling rate: faster cooling in the smaller mold resulted in a lower crystal number density and a reduced crystallized volume fraction (αv) as expected; ii) mold material: surprisingly, copper molds led to quicker glass shrinkage, which facilitated the earlier formation of air gaps with reduced heat transfer and slower cooling than steel, favoring incipient crystallization during the cooling path; iii) microstructure: samples cooled in both molds exhibited higher αv in the central and upper (mold contact-free) regions due to slower cooling compared to the mold base and edges. Therefore, this study reveals how mold material and size affect microstructural gradients in GCs, paving the way for tailoring crystallization and microstructure through strategic mold design.