DOE OSTI2017
Fuel cladding chemical interactions (FCCI) have been acknowledged as a critical issue in a metallic fuel/steel cladding system due to the formation of low melting intermetallic eutectic compounds between the fuel and cladding steel, resulting in reduction in cladding wall thickness as well as a formation of eutectic compounds that can initiate melting in the fuel at lower temperature. In order to mitigate FCCI, diffusion barrier coatings on the cladding inner surface have been considered. In order to generate the required coating techniques, pack cementation, electroplating, and electrophoretic deposition have been investigated. However, these methods require a high processing temperature of above 700 oC, resulting in decarburization and decomposition of the martensites in a ferritic/martensitic (F/M) cladding steel. Alternatively, organometallic chemical vapor deposition (OMCVD) can be a promising process due to its low processing temperature of below 600 oC. The aim of the project is to conduct applied and fundamental research towards the development of diffusion barrier coatings on the inner surface of F/M fuel cladding tubes. Advanced cladding steels such as T91, HT9 and NF616 have been developed and extensively studied as advanced cladding materials due to their excellent irradiation and corrosion resistance. However, the FCCI accelerated by the elevated temperature and high neutron exposure anticipated in fast reactors, can have severe detrimental effects on the cladding steels through the diffusion of Fe into fuel and lanthanides towards into the claddings. To test the functionality of developed coating layer, the diffusion couple experiments were focused on using T91 as cladding and Ce as a surrogate lanthanum fission product. By using the customized OMCVD coating equipment, thin and compact layers with a few micron between 1.5 µm and 8 µm thick and average grain size of 200 nm and 5 µm were successfully obtained at the specimen coated between 300oC and 500 oC, respectively. The coating layer contains both carbon and vanadium elements as quantified by WED, and the phases mainly consist of a mixture of V2C and VC, which was confirmed using X-ray diffraction patterns. In addition, the ratio between V and C varies with processing temperature, and it was observed that a higher temperature promotes the carbon adsorption and increases thickness of the coating. With optimized deposition conditions, we can apply the coating technique toward the actual T91 cladding materials, and provide the possibilities for the real application in sodium-cooled fast reactors (SFRs). Diffusion couple experiments were performed at both 550 oC and 690 oC, which corresponds to normal and aggressive operating temperatures, respectively. The results show that vanadium carbide coating with wider thickness (8 µm) and lower carbon concentration (27 at.%) reduced the width of the inter diffusion region, indicating that vanadium carbide coating can mitigate FCCI effectively. In specific, inter-diffusion between Fe and Ce was prohibited over most area, but Ce diffusion occurred toward the coating and the Fe substrate through thinner coating layer, which needs further optimization in terms of uniform coating thickness. Overall, it is concluded that this coating process can be successfully applied onto the inner surface of HT9 cladding tubes and the FCCI can be effectively mitigated if not totally eliminated.