Microstructural Observations on Advanced Multilayer Protective Coatings for Nuclear Thermal Propulsion

The present research discusses the microstructures of a new multilayered coating concept proposed to solve the “midrange corrosion” problem observed in NbC and ZrC-coated graphite (Gr) nuclear fuels during the NERVA/Rover programs. The concept envisions designing a compliant multilayered coatings architecture to accommodate the thermal expansion mismatch strains between the ZrC outer coating and the Gr/(U,Zr)C fuel matrix along with using a diffusion barrier to minimize carbon and hydrogen diffusion, respectively. Multilayered coatings were deposited on Gr substrates by chemical vapor deposition (CVD). Graphite disks, as well as the inner channels of a 19-hole hexagonal rod 152.4 mm long, were coated by CVD in proof-of concept process demonstration studies. Coated disk specimens were thermally-cycled between ambient and 1900 K for as long as 20 cycles with a 1h hold time at the temperature using both stepped and non-interrupted thermal cycling methods. Detailed cross-sectional microstructural analyses were conducted on the thermally-cycled coated disks. These results showed that the coatings were intact after 20 thermal cycles at 1900 K although the bonding of the overlay Mo coating appeared to be influenced by the oxygen content in the layer. Seven transverse sections were cut along the length from the coated hexagonal rod for microstructural studies. All the nineteen channels were observed to have been coated in all the sections. This paper reports the results of detailed microstructural analyses, compositional line scans and x-ray dot maps conducted on three coated channels from a mid-section of the rod. The measured values of carbon (C) were observed to be exceptionally high in all the specimens, which were attributed to hydrocarbon contamination of the specimen surfaces. It was observed that the oxygen (O) levels were high in all the coating layers even after approximately correcting for the observed high values of C. The source of O contamination of the CVD reactor system was attributed to either the presence of oxychloride impurities in the precursor salts or a pin hole leak in the coating system. It is concluded that high values of O result in poor bonding of the Mo overlay to the ZrC layer. These trials have established that it is possible to deposit multilayered coatings by CVD in 19-hole hexagonal rods 152.4 mm long similar to the NERVA fuel rod design although the quality of the coatings and the uniformity of their thicknesses require further improvement.