Effects of crystal structure and cation size on molten silicate reactivity with environmental barrier coating materials

Rare earth (RE) disilicates are utilized in environmental barrier coatings to protect Si-based engine components from destructive reactions with water vapor and other combustion species. These coating materials, however, degrade when exposed to molten silicate deposits in the engine. Four RE-disilicates (RE2Si2O7, RE = Er, Dy, Gd, Nd) are analyzed herein in thermochemical interactions with glassy calcium-magnesium-aluminosilicate (CMAS) compositions at 1400 degrees C. Crystalline reaction products included RE2Si2O7, SiO2, and a Ca2+yRE8+x(SiO4)(6)O-2+3(x)/2+(y) apatite-type silicate. RE2Si2O7 formation was favored in interactions with CMAS having low CaO:SiO2 ratios. Increased reactivity was observed for higher CaO:SiO2 ratios in CMAS combined with larger RE3+ cation size, resulting in apatite formation of varying stoichiometry and changes in lattice parameters. The crystallization of SiO2 was dependent on both thermodynamic equilibrium at low CaO:SiO2 ratios and sequestration of silicate modifiers at higher CaO:SiO2 ratios, although residual amorphous content after CMAS exposure in both cases was still substantial.