[en] In a scenario of aqueous transport from a high-level radioactive waste repository, the concentration of radionuclides in water in contact with the waste constitutes the source term for transport models, and as such represents a fundamental component of all performance assessment models. Many laboratory experiments have been done to characterize release rates and understand processes influencing radionuclide release rates from irradiated nuclear fuel. Natural analogues of these waste forms have been studied to obtain information regarding the long-term stability of potential waste forms in complex natural systems. This information from diverse sources must be brought together to develop and defend methods used to define source terms for performance assessment models. In this manuscript examples of measures of radionuclide release rates from spent nuclear fuel or analogues of nuclear fuel are presented. Each example represents a very different approach to obtaining a numerical measure and each has its limitations. There is no way to obtain an unambiguous measure of this or any parameter used in performance assessment codes for evaluating the effects of processes operative over many millennia. The examples are intended to suggest by example that in the absence of the ability to evaluate accuracy and precision, consistency of a broadly based set of data can be used as circumstantial evidence to defend the choice of parameters used in performance assessments

[en] A report on the immobilization of uranium in the earth's crust has been completed. Techniques have been developed to do a comprehensive mass inventory of the Oklo reactor zones. These techniques were applied to a compilation of data from Oklo zones 2 and 3-4. The study shows large deficiencies of neodymium, ruthenium, and mass 99 elements (⁹⁹Tc or ⁹⁹Ru) in the reactor zones. The extent of these deficiencies are correlated with the intensity of the nuclear reactions. Analyses of ores from the Key Lake uranium mineralization show that 60 to 70% of the radiogenic lead is missing from the ores

No abstract available

[en] An interim report has been published on the redistribution of uranium, thorium, and lead in samples representing several million cubic meters of sandstone and metamorphosed sediments in the Athabasca Basin which is located in the northwest corner of the Canadian province of Saskatchewan. The region of study includes zones of uranium mineralization at Key Lake. Mineralization occurs at the unconformity between the Athabasca sandstone and the underlying metasediments and in fault zones within the metasediments. Lead isotopes record a radiometric age of 1300 +- 150 m.y. in samples from above and below the unconformity. This age probably reflects the time of deposition of the sandstones and an associated redistribution of uranium and/or lead in the underlying rocks. Many of the samples have been fractionated with respect to radiogenic lead and the actinide parent elements since that time. Sandstones and altered rocks from the region above the unconformity have been a transport path and are a repository for lead. In contrast, mineralized rocks are deficient in radiogenic lead and must be an important source of lead in the local geologic environment. Samples from Oklo reactor zone 9 and nearby host rocks have been prepared for isotopic analyses of ruthenium, molybdenum, uranium and lead

[en] Lead and uranium isotopic abundances in rocks from the Oklo mine show large deficiencies of radiogenic lead in the mineralized regions and enormous excesses of this element outside the uraniferous zones. A fracture lined with secondary minerals and its host rock from distances as far as approx. 13 meters away contain lead that was deposited contemporaneously. The isotopic composition of lead in these samples varies systematically as a function of distance from the fracture. This regularity may reflect the nature of the processes that transported lead from the ores and deposited it in the surrounding rocks

[en] The final draft of a paper entitled The Oklo Reactors: Natural Analogs to Nuclear Waste Repositories has been submitted for publication. This paper discusses the chemical stability of the fossil reactors with respect to uranium, neodymium, ruthenium, and technetium, the transport of elements in the geologic environment at Oklo; and the geochemical conditions that may have influenced these processes. Measurements of barium isotopic ratios limit the abundance of fissiogenic barium to <10^-7 g/g and <2 x 10^-6 g/g in two samples peripheral of Oklo reactor zone 9. Samples from the Oklo mines have been sent to Australia for cooperative studies on the geochemistry of palladium, silver, cadmium, tin, and tellurium. Four samples representing a traverse to the east of reactor zone 9 are being analyzed to determine the isotopic composition of molybdenum and ruthenium

[en] Samples from Oklo Reactor zone-9 (ORZ-9) have been analyzed for the isotopic abundances of Nd, Ce, Ru, and Mo. Interpretation of the Nd data has begun as part of the effort to reconstruct the operating parameters of the reactor. The study of ORZ-9 and the peripheral rocks is being enhanced by additional analytical capabilities. A procedure was developed to measure uranium isotopic ratios with high precision. This new method was used for the analysis of rocks peripheral to ORZ-9. Two rocks containing relatively small quantities of uranium were depleted in ²³⁵U. The result demonstrates that small quantities of uranium were removed from the reactor zone and redistributed over distances of several tens of meters. Procedures are being designed to make high precision measurements of the relative abundances of barium isotopes. They will be used as part of a study of the transport of alkali and alkaline earth elements at Oklo. Samples from distances up to 300 meters from the known mineralized area at Oklo have been selected and prepared in an effort to identify element transport paths over longer distances. A sample from the Athabasca sandstone, overlying the uranium ores at Key Lake, and another from the transition zone at the unconfromity between the sandstone and the basement were subjected to sequential leaches designed to preferentially dissolve specific minerals. Lead isotopic analyses on the leachs yielded two sets of data, which indicate the loss of uranium or the addition of lead from a radiogenic source early in the geologic history of the rocks

[en] The unique isotopic composition of lead from uranium ores can be useful in studying the impact of ore processing effluents on the environment. Common lead on the earth's surface is composed of 1.4% ²⁰⁴Pb, 24.1% ²⁰⁶Pb, 22.1% ²⁰⁷Pb, and 52.4% ²⁰⁸Pb. In contrast, lead associated with young uranium ores may contain as much as 95% ²⁰⁶Pb. These extreme differences provide the means to quantitatively evaluate the amount of lead introduced into the environment from the mining and milling of uranium ores by measuring variations of the isotopic composition of lead in environmental samples. The use of Pb isotopes as diagnostic tools in studying the hydrologic transport of materials from U ore dressing plants in the Grants Mineral Belt, New Mexico, is discussed. Preliminary measurements on effluents intimately associated with processing wastes are consistent with a simple model in which radiogenic lead from the ores is mixed with common lead from the uncontaminated environments

[en] U-Pb and Pb isotopic data are presented which indicate that Pb is lost from host uraninite by diffusion, and that not only in situ uranogenic Pb but also the initial Pb is lost by diffusion. The conglomerate underlying the U deposit contains excess Pb and is both a transport zone and the repository for the Pb. 2 figures

[en] The redistribution of uranium, thorium, and lead is being examined in samples representing several million cubic meters of sandstone and metamorphased sediments in the Athabasca Basin which is located in the northwest corner of the Canadian province of Saskatchewan. The region of study includes zones of uranium mineralization at Key Lake. Mineralization occurs at the unconformity between the Athabasca sandstone and the underlying metasediments and in fault zones within the metasediments. Lead isotopes record a radiometric age of 1300 +- 150 m.y. in samples from above and below the unconformity. This age probably reflects the time of deposition of the sandstones and an associated redistribution of uranium and/or lead in the underlying rocks. Many of the samples have been fractionated with respect to radiogenic lead and the actinide parent elements since that time. Sandstones and altered rocks from the region above the unconformity have been a transport path and are a repository for lead. In contrast, mineralized rocks are deficient in radiogenic lead and must be an important source of lead in the local geologic environment. However, the isotopic composition of lead missing from the ores is different from that found in the overlying sandstones. The two types of rocks do not appear to represent complements with respect to a source and a repository for lead