Oxide Growth and Validation for Aluminum Research Reactor Fuel - 19422
Aluminum fuel cladding will undergo general corrosion with resulting formation of adherent oxide films during in-reactor and post-discharge exposures under various water conditions and temperatures. These oxides include chemically-bound water that can pose challenges for extended dry storage. This paper describes laboratory experiments performed to produce hydroxide (oxide) films on aluminum 1100, 6061 and 5052 series alloy substrates immersed in water at controlled temperatures. The results are compared to the oxide film present on a spent fuel assembly irradiated in research reactor. This work is part of a broad investigation to address knowledge gaps and technical data needs for dry storage of aluminum-clad spent nuclear fuel (SNF). To adequately assess the risks posed by chemically-bound water on SNF in dry storage and strategies for removing chemically bound water, it is necessary to understand the expected composition and loading of oxide films on SNF of different service histories and to investigate the response of such oxides to irradiation and potential drying methods. These efforts require both the growth of films under controlled conditions and the production of non-radioactive surrogates for testing. The current work comprises experimental investigation of oxide growth via (1) laboratory experiments to produce hydroxide films on aluminum alloy substrates immersed in water at controlled temperatures and (2) characterization and comparison of laboratory-grown oxides to oxides on service-exposed aluminum alloys. The important factors affecting oxide growth and characteristics typical of oxide films formed by aqueous corrosion under conditions similar to in-reactor are reviewed. Aluminum oxide films were grown under a variety of controlled temperature conditions and durations to serve as surrogates for oxides found on aluminum-clad spent nuclear fuel due to aqueous corrosion. The chemically-bound water found in oxides formed by aqueous corrosion poses challenges for extended dry storage, requiring investigation of how the oxide loading and characteristics vary with exposure history and to provide the initial condition for investigation of drying methods. Characteristics including chemical composition, oxide morphology, and film thickness were measured to assess whether the surrogate films were representative of in-service-produced oxides on SNF. Tests were conducted in liquid water at atmospheric pressure in the temperature range 50-100 deg. C, with and without heat flux through the corroding surface, to replicate in-service conditions, and at 185 deg. C inside pressure vessels to replicate pre-filming procedures. Three different alloys commonly used in aluminum clad research reactor fuel were considered: Al-1100, Al-6061, and Al-5052. Specimens were characterized by weighing before and after exposure to measure oxide mass loading, X-ray diffraction to identify oxide composition, and scanning electron microscopy to examine the oxide morphology and film thickness. The oxide type and the morphological characteristics of the film on a fuel element from the Uruguay RU1 research reactor were determined and compared to the laboratory surrogates. The results show some differences compared to the 50 deg. C laboratory specimen that are rationalized with the service storage history of the element. (authors)