Thermal barrier coatings (TBCs) are increasingly susceptible to degradation by molten calcium-magnesium alumino silicate (CMAS) deposits in advanced engines that operate at higher temperatures and in environments laden with siliceous debris. This paper investigates the thermochemical aspects of the degradation phenomena using a model CMAS composition and ZrO 2 -7.6%YO 1.5 (7YSZ) grown by vapor deposition on alumina substrates. The changes in microstructure and chemistry are characterized after isothermal treatments of 4 h at 12001-14001C. It is found that CMAS rapidly penetrates the open structure of the coating as soon as melting occurs, whereupon the original 7YSZ dissolves in the CMAS and reprecipitates with a different morphology and composition that depends on the local melt chemistry. The attack is minimal in the bulk of the coating but severe near the surface and the interface with the substrate, which is also partially dissolved by the melt. The phase evolution is discussed in terms of available thermodynamic information.

Molten deposits based on calcium-magnesium alumino-silicates (CMAS), originating from siliceous debris ingested with the intake air, represent a fundamental threat to progress in gas turbine technology by limiting the operating surface temperature of coated components. The thermomechanical and thermochemical aspects of the CMAS interactions with thermalbarrier coatings, as well as the current status of mitigating strategies, are discussed in this article. Key challenges and research needs for developing adequate solutions are highlighted.

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The temperature capability of yttria-stabilized zirconia thermal barrier coatings (TBCs) is ultimately tied to the rate of evolution of the ''nontransformable'' t 0 phase into a depleted tetragonal form predisposed to the monoclinic transformation on cooling. The t 0 phase, however, has been shown to decompose in a small fraction of the time necessary to form the monoclinic phase. Instead, a modulated microstructure consisting of a coherent array of Y-rich and Y-lean lamellar phases develops early in the process, with mechanistic features suggestive of spinodal decomposition. Coarsening of this microstructure leads to loss of coherency and ultimately transformation into the monoclinic form, making the kinetics of this process, and not the initial decomposition, the critical factor in determining the phase stability of TBCs. Transmission electron microscopy is shown to be essential not only for characterizing the microstructure but also for proper interpretation of X-ray diffraction analysis.

Phase evolution accompanying the isothermal aging of free‐standing air‐plasma sprayed (APS) 7–8 wt% yttria‐stabilized zirconia (8YSZ) thermal barrier coatings (TBCs) is described. Aging was carried out at temperatures ranging from 982°C to 1482°C in air. The high‐temperature kinetics of the phase evolution from the metastable t′ phase into a mixture of transformable Y‐rich (cubic) and Y‐lean (tetragonal) phases are documented through ambient temperature X‐ray diffraction (XRD) characterization. A Hollomon–Jaffe parameter (HJP), T[27 + ln(t)], was used to satisfactorily normalize the extent of phase decomposition over the full range of times and temperatures. Comparison to vapor deposited TBCs reveal potential differences in the destabilization mechanism in APS coatings. Furthermore, the lattice parameters extracted from Rietveld refinement of the XRD patterns were used to deduce the stabilizer concentrations of the respective phases, which suggest a retrograde tetragonal solvus over the temperature range studied. In concert with a complementary microstructural study presented in Part II, this effort offers new insights into the mechanisms governing the phase evolution and raises implications for the high‐temperature use of 8YSZ ceramics.

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