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Glass strategy: Hanford’s enhanced waste glass program
The mission of the Department of Energy’s Office of River Protection (ORP) is to complete the safe cleanup of waste resulting from decades of nuclear weapons development. One of the most technologically challenging responsibilities is the safe disposition of approximately 56 million gallons of radioactive waste historically stored in 177 tanks at the Hanford Site in Washington state.
ORP has a clear incentive to reduce the overall mission duration and cost. One pathway is to develop and deploy innovative technical solutions that can advance baseline flow sheets toward higher efficiency operations while reducing identified risks without compromising safety. Vitrification is the baseline process that will convert both high-level and low-level radioactive waste at Hanford into a stable glass waste form for long-term storage and disposal.
Although vitrification is a mature technology, there are key areas where technology can further reduce operational risks, advance baseline processes to maximize waste throughput, and provide the underpinning to enhance operational flexibility; all steps in reducing mission duration and cost.
Steven D. Herrmann, Brian R. Westphal, Shelly X. Li, Haiyan Zhao
Nuclear Technology | Volume 208 | Number 5 | May 2022 | Pages 871-891
Technical Paper | doi.org/10.1080/00295450.2021.1973180
Articles are hosted by Taylor and Francis Online.
Prior work identified dissolution of used nuclear oxide fuel constituents from a uranium oxide matrix into molten LiCl-KCl-UCl3 at 500°C, prompting a subsequent series of three progressive studies (including an initial scoping study, an electrolytic dissolution study, and a chemical-seeded dissolution study) to further investigate associated parameters and mechanisms. Thermodynamic calculations were performed to identify possible reaction mechanisms and their propensities in used oxide fuel constituent dissolution. Used nuclear oxide fuels with varying preconditions from fast and thermal test reactors were separately immersed in the subject salt system to assess fuel constituent migration from the bulk fuel matrix to the salt phase in an initial scoping study. Dissolution of expected fuel constituents, including alkali, alkaline earth, lanthanide, and transuranium oxides, into the chloride salt phase varied widely, ranging from 12% to 99% in the initial study. Uranium isotope blending between the salt phase and bulk fuel matrix was also observed, which was attributed to reducing conditions in the fuel matrix. Electrolytic and chemical-seeded dissolution studies were subsequently performed to effect reducing conditions in the fuel. Other parameters, including temperature (at 500°C, 650°C, 725°C, and 800°C) and uranium trichloride concentrations (at 6, 9, and 19 wt% uranium), were investigated in the latter two studies, resulting in fuel constituent dissolution above 90%. Extents of dissolution were based on initial and final fuel constituent concentrations in the oxide fuels following operations in the salt and subsequent removal of the salt via distillation. In this series of progressive studies, oxide fuel preconditioning and in situ reducing conditions, along with elevated temperature and uranium trichloride concentrations, were the primary parameters promoting used nuclear oxide fuel constituent dissolution in accordance with identified reaction mechanisms.