Combinatorial processing and evaluation of the phase evolution and oxidation behavior of Hf-Al-Si refractory complex concentrated alloys

Abstract

Refractory complex concentrated alloys (RCCAs) are a unique group of materials defined by the shared principality between all alloying elements and the tailorable properties at high temperatures (>1000 °C). RCCA systems can be optimized using high-throughput processing which allows for simultaneous characterization and testing over a range of compositions. A compositionally-graded Hf-Al-Si coating was compositionally mapped using scanning electron microscopy (SEM) with energy dispersive spectroscopy (EDS) to identify relative compositions as a function of position on the wafer. High temperature CALPHAD phase diagrams and thermodynamic predictions for a Hf50Al50-xSix alloy and its (Hf50Al50-xSix)1-yOy oxide were coupled with experimental results. The RCCA wafer was heat treated at 1200 °C to observe any phase changes and oxidation behavior at elevated temperatures. Characterization of the RCCA was performed before and after heating using synchrotron radiation X-ray diffraction (SR-XRD) to identify the phases and oxidation states as a function of the compositional gradient and to determine an alloy composition range with the least oxidation. SR-XRD pre- and post-treating revealed an inherent amorphous Hf20Al7Si13 phase across the as-deposited coating, similarities in spectra pre- and post-treating for compositions containing less Hf and more Al and Si relative to the entire gradient film, and the presence of significant HfO2 and Al6Si2O13 oxide for compositions consisting of more Hf and less Al and Si relative to the entire gradient film. The SR-XRD and CALPHAD modeling suggests that compositions of 31–48 at.% Hf, 21–48 at.% Al, and 9–27 at.% Si display the greatest resistance to detrimental oxidation upon heating to 1200 ∘C.