Microstructure evolution in amorphous Hf-B-Si-C-N high temperature resistant coatings after annealing to 1500 °C in air

Recently, amorphous Hf-B-Si-C-N coatings found to demonstrate superior high-temperature oxidation resistance. The microstructure evolution of two coatings, Hf7B23Si22C6N40 and Hf6B21Si19C4N47, annealed to 1500 degrees C in air is investigated to understand their high oxidation resistance. The annealed coatings develop a two-layered structure comprising of the original as-deposited film followed by an oxidized layer. In both films, the oxidized layer possesses the same microstructure with HfO2 nanoparticles dispersed in an amorphous SiOx-based matrix. The bottom layer in the Hf6B21Si19 C4N47 coating remains amorphous after annealing while Hf7B23Si22C6N40 recrystallized partially showing a nanocrystalline structure of HfB2 and HfN nanoparticles separated by h-Si3N4 and h-BN boundaries. The HfB2 and HfN nanostructures form a sandwich structure with a HfB2 strip being atomically coherent to HfN skins via (111)-Hf monolayers. In spite of the different bottom layer structure, the oxidized/bottom layer interface of both films was found to exhibit a similar microstructure with a fine distribution of HfO2 nanoparticles surrounded by SiO2 quartz boundaries. The high-temperature oxidation resistance of both films is attributed to the particular evolving microstructure consisting of HfO2 nanoparticles within a dense SiOx-based matrix and quartz SiO2 in front of the oxidized/bottom layer interface acting as a barrier for oxygen and thermal diffusion.