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Methods for forming high temperature coating systems (34) are provided, as are gas turbine engine components (10) including such coating systems. In embodiments, the coating formation method includes forming a fracture-resistant Thermal Barrier Coating (TBC) layer (42) over a component surface (36). The fracture-resistant TBC layer (42) is produced from a first coating precursor material containing an amount of zirconia in mole percent (ZrOmol%1) and an amount of tantala in mole percent (TaOmol%1). A Calcium-Magnesium Aluminosilicate (CMAS) resistant TBC layer (44) is formed over the fracture-resistant TBC layer (42) from a second coating precursor material, which contains an amount of zirconia in mole percent (ZrOmol%2), an amount of tantala in mole percent (TaOmol%2), and an amount of one or more rare earth oxides in mole percent (REOmol%2). The first and second coating precursor materials are formulated such that ZrOmol%1 is greater than ZrOmol%2, TaOmol%1 is less than TaOmol%2, and TaOmol%2 is substantially equivalent to REOmol%2.