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The evaluated spectroscopic data are presented for known nuclides of mass 228 (Ac, At, Fr, Np, Pa, Pu, Ra, Rn, Th, and U). Excited states in {sup 228}At, {sup 228}Rn, {sup 228}Fr, {sup 228}Np, and {sup 228}Pu have not been identified as yet. Significant amounts of new data have been added since the last evaluation of A=228 nuclides. This work supersedes earlier full evaluations of A=228 published by 1997Ar08.
The nucleus {sup 235m}U is an isomer with extremely low excitation energy (76.8 eV) and decays dominantly through the internal conversion (IC) process. Because outer-shell electrons are involved in the IC process, the decay constant of {sup 235m}U depends on its chemical environment. We plan to study the deexcitation process of {sup 235m}U by measuring the energy spectra of IC electrons in addition to the decay constants for various chemical forms. In this paper, the preparation method of {sup 235m}U samples from {sup 239}Pu by using alpha-recoil energy is reported. A Collection Apparatus for Recoil Products was fabricated, and then collection efficiencies under various conditions were determined by collecting {sup 224}Ra recoiling out of {sup 228}Th electrodeposited and precipitated sources. The pressure in the apparatus (vacuum or 1 atm of N{sub 2} gas) affected the variations of the collection efficiencies depending on the negative voltage applied to the collector. The maximum values of the collection efficiencies were mainly affected by the thickness of the {sup 228}Th sources. From these results, the suitable conditions of the {sup 239}Pu sources for preparation of {sup 235m}U were determined. In addition, dissolution efficiencies were determined by washing collected {sup 224}Ra with solutions. When {sup 224}Ra was collected in 1 atm of N{sub 2} gas and dissolved with polar solutions such as water, the dissolution efficiencies were nearly 100%. The method of rapid dissolution of recoil products would be applicable to rapid preparation of short-lived {sup 235m}U samples for various chemical forms.
An Evaluation and Screening (E and S) study of nuclear fuel cycle options was recently conducted for the U.S. Department of Energy to identify promising fuel cycle options with the potential for achieving substantial improvements compared to the current nuclear fuel cycle in the U.S. This study considered the entire fuel cycle, i.e., the complete nuclear energy system from mining to disposal including both once-through and recycle fuel cycles. The E and S study considered performance at steady-state when evaluating the potential benefits and challenges to achieving that eventual end state. Based on the steady-state findings from the E and S, a set of four fuel cycle options (FCOs) were identified as most promising, in terms of offering the most benefits compared to the current cycle. These FCOs have natural uranium (or existing stocks of uranium such as depleted uranium) as the makeup feed sent to the fast reactor (FR) fleet combined with two dimensions. The first dimension is whether the FR is a single-stage (produces just enough fuel resources to sustain operation and growth of the FR fleet) or a two-stage (produces additional fuel resources to also sustain a companion fleet of thermal reactors) fuel cycle. In all four cases, all of the uranium is continuously recycled. The second dimension is whether only the plutonium is co-extracted and recycled with the uranium (with minor actinides disposed as waste) or all transuranic elements are co-extracted and recycled. The four most promising options are: 1) single-stage FR recycling of U/Pu (EG23), 2) recycling of U/TRU in single-stage FR (EG24), 3) recycling of U/Pu in two-stage FR/thermal reactors (EG29), and 4) recycling of U/TRU in two-stage FR/thermal reactors (EG30). (authors)
As described in companion papers, Westinghouse is proposing the implementation of a thorium based fuel cycle to burn the transuranic (TRU) contained in the used nuclear fuel. The potential of thorium as a TRU burner is described in another paper presented at this conference. This paper analyzes the long-term impact of thorium on the front-end and backend of the fuel cycle. This is accomplished by an assessment of the isotopic make-up of Th in a closed cycle and its impact on representative metrics, such as radiotoxicity, decay heat and gamma heat. The behavior in both thermal and fast neutron energy ranges has been investigated. Irradiation in a Th fuel PWR has been assumed as representative of the thermal range, while a Th fuel fast reactor (FR) has been employed to characterize the behavior in the high-energy range. A comparison with a U-fuel closed-cycle FR has been undertaken in an attempt of a more comprehensive evaluation of each cycle's long-term potential. As the Th fuel undergoes multiple cycles of irradiation, the isotopic composition of the recycled fuel changes. Minor Th isotopes are produced; U-232 and Pa-231 build up; the U vector gradually shifts towards increasing amounts of U-234, U-235 etc., eventually leading to the production of non negligible amounts of TRU isotopes, especially Pu-238. The impact of the recycled fuel isotopic makeup on the in-core behavior is mild, and for some aspects beneficial, i.e. the reactivity swing during irradiation is reduced as the fertile characteristics of the fuel increase. On the other hand, the front and the back-end of the fuel cycle are negatively affected due to the presence of Th-228 and U-232 and the build-up of higher actinides (Pu-238 etc.). The presence of U-232 can also be seen as advantageous as it represents an obstacle to potential proliferators. Notwithstanding the increase in the short-term radiotoxicity and decay heat in the multi-recycled fuel, the Th closed cycle has some potentially substantial advantages compared to the U cycle, such as the smaller actinide radiotoxicity and decay heat for up to 25,000 years after irradiation. In order for these benefits to materialize, the capability to reprocess and remotely manufacture industrial amounts of recycled fuel appears to be the key. Westinghouse is proposing the implementation of a thorium based fuel cycle to burn the TRU contained in the current UNF. The general approach and the potential of thorium as TRU burner is described in other papers presented at this conference. The focus of this paper is to analyze the long-term potential of thorium, once the legacy TRU has been exhausted and the thorium reactor system will become self-sufficient. Therefore, a comparison of Th closed cycle, in fast and thermal neutron energy ranges, vs. U closed cycle, in the fast energy range, has been undertaken. The results presented focus on selected backend and front-end metrics: isotopic actinide composition and potential implications on ingested radiotoxicity, decay heat and gamma heat. The evaluation confirms potential substantial improvements in the backend of the fuel cycle by transitioning to a thorium closed cycle. These benefits are the result of a much lower TRU content, in particular Pu-241, Am-241 and Pu-240, characterizing the Th vs. U actinide inventories, and the ensuing process waste to be disposed. On the other hand, the larger gamma activity of Th recycled fuel, consisting predominantly of hard gammas from U-232's decay products, is a significant challenge for fuel handling, transportation and manufacturing but can be claimed as beneficial for the proliferation resistance of the fuel. It is worth remembering that in our perspective the Th closed cycle and the U closed cycle will follow a transmutation phase which will likely take place over several decades and dictate the technologies required. These will likely include remote fuel manufacturing, regardless of the specific system adopted for the transmutation, which could then be inherited for the ensuing closed cycles. Finally, specific data related to the fuel manufacturing and separation technologies and their performance in the prospected industrial scale deployment, are key for further quantification of the potential merits of the options explored. Further studies in this direction should be warranted before making definitive conclusion. (authors)