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Hartmann, T.; Paviet-Hartmann, P.; Wetteland, C.J.; Lu, N.; Ware, S.D.; Sage, S.
Los Alamos National Laboratory (United States). Funding organisation: US Department of Energy (United States)2002
Los Alamos National Laboratory (United States). Funding organisation: US Department of Energy (United States)2002
AbstractAbstract
[en] In the event of inundation of a nuclear waste repository located in a geological salt formation, chloride brines in contact with nuclear waste will be exposed to different kind of radiation depending on waste-form conditions. Ionizing radiations, however, have the ability to significantly affect the groundwater chemistry of the brines through the formation of free radicals, ionic- and molecular species; among them the typical byproducts of a-radiolysis: hypochlorite (OC1-) and hypochlorous acid (HOCl). In the absence of effects which arc supposed to dominate the redox conditions in the repository (corrosion of metals, microbial activity) the presence of OC1- is known to increase the redox potential of the brines and further to influence the stability of actinide waste-forms by accelerating their dissolution arid - most importantly - to oxidize actinides to their higlier oxidation states, whicli are gcncrally the most soluble ones. We are presenting a new approach to determine the radiation-induced formation rates of hypochlorite and hypochlorous acid as a first step to assess long-term steady-state repository conditions. To ovt:rcome the serious constraints of conventional radiocheinical work with GBq activity levels, we are simulating a-irradiation of chloride brines by the adaptation of ion-beam-line experiments. Therefore, we irradiate liquid chloride brine targets with 5 MeV protons, and 5 MeV helium ions. The irradiation-induced formation rates of OCX- and HOC1 were determined by UV-Vis spectrophotometry. To give an example, the measured G values for the HOCl formation in 3.7 M MgC12.6H20, pW 4.42, irradiated by 5 MeV protons was determined to be 0.0374 ± 0.0022, and 0.0536 ± 49 by irradiating with 5 MeV helium. The distinguished ltnowledge about the radiation-induced production of oxo-chloride species is the first step towards the assumption of their steady-state concentrations in the irradiation field of the repository.
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1 Jan 2002; 9 p; MRS 2002 Fall Meeting; Boston, MA (United States); 2-6 Dec 2002; Available from http://lib-www.lanl.gov/cgi-bin/getfile?00855519.pdf; PURL: https://www.osti.gov/servlets/purl/976387-xPAjwS/
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