scholarly journals Report on Intact and Degraded Criticality for Selected Plutonium Waste Forms in a Geologic Repository, Volume I: MOX SNF

1998 ◽  
Author(s):  
J.A. McClure
2000 ◽  
Vol 6 (S2) ◽  
pp. 368-369
Author(s):  
N.L. Dietz ◽  
D.D Keiser

Argonne National Laboratory has developed an electrometallurgical treatment process for metallic spent nuclear fuel from the Experimental Breeder Reactor-II. This process stabilizes metallic sodium and separates usable uranium from fission products and transuranic elements that are contained in the fuel. The fission products and other waste constituents are placed into two waste forms: a ceramic waste form that contains the transuranic elements and active fission products such as Cs, Sr, I and the rare earth elements, and a metal alloy waste form composed primarily of stainless steel (SS), from claddings hulls and reactor hardware, and ∼15 wt.% Zr (from the U-Zr and U-Pu-Zr alloy fuels). The metal waste form (MWF) also contains noble metal fission products (Tc, Nb, Ru, Rh, Te, Ag, Pd, Mo) and minor amounts of actinides. Both waste forms are intended for eventual disposal in a geologic repository.


1987 ◽  
Vol 112 ◽  
Author(s):  
B. Grambow ◽  
D. M. Strachan

The reprocessing of spent fuel from nuclear reactors and processing of fuels for defense purposes have generated large volumes of high-level liquid waste that need to be immobilized prior to final storage. For immobilization, the wastes must be converted to a less soluble solid, and, although other waste forms exist, glass currently appears to be the choice for the transuranic-containing portion of the reprocessed waste. Once produced, this glass will be sent in canisters to a geologic repository located some 200 to 500 m below the surface of the earth.


1987 ◽  
Vol 112 ◽  
Author(s):  
Susan L. Hoyle ◽  
Michael W. Grutzeck

AbstractRecent work by the authors has demonstrated that cesium was being incorporated in a hydrated phase as their cement-based waste forms cured. The objective of the present study was to identify the hydrated phases responsible for the observed cesium incorporation. Four calcium aluminosilicate glasses having a 1:2 Al2O3/CaO ratio and a 25–70 mole % silica content were mixed with ˜0.3 molar CsOH or CsCl solutions (water/solid ratio = 10) and allowed to hydrate at 38° and 90°C for periods up to 90 days. Paste equivalent samples, having a water/solid ratio of 1.0 were also prepared to gauge the cementing properties of these mixtures. Solutions were analyzed for Ca, Al, Si, and Cs while solids were characterized using x-ray powder diffraction and scanning electron microscopy.Glasses exposed to the CsOH solution were more reactive than their counterparts exposed to the CsCl solution. In addition, reactivity as well as crystallinity seemed to be higher at 90° than at 38°C. At least two cesium-containing zeolites were identified in the 90°C CsOH solution experiment: A cesium-containing wairarkite analogue and possibly another cesium-containing zeolite unidentified at this time. The relatively complete removal of cesium from the solution, in one case, as well as the fact that the mixtures are self-cementing suggests that the glasses may be “engineered” to serve as overpack material in a deep-seated geologic repository.


1983 ◽  
Vol 26 ◽  
Author(s):  
Thomas H. Pigford

ABSTRACTThis study was conducted for the U. S. Department of Energy by the Waste Isolation Systems Panel appointed by the National Academies of Science and Engineering. The panel was charged to review the alternative technologies available for Isolating of radioactive waste in mined geologic repositories, evaluate the performance benefits from these technologles as potential elements of a waste Isolation system, and identify appropriate technical criteria for satisfactory long-term performance of a geologic repository. Conceptual repositories in basalt, granite, salt, and tuff were considered. Site-specific data on geology, hydrology, and geochemical properties were evaluated and used to define parameters for estimating long-term environmental releases, supplemented when necessary by generic properties.The technology for solid waste forms and waste packages was reviewed and evaluated. Borosilicate glass and unreprocessed spent fuel are the waste forms appropriate for further testing and for repository designs. Testing in a simulated repository environment is necessary to develop an adeauate prediction of the long term performance of waste packages in a geologic repository. Back-up research and development on alternative waste forms should be continued. The expected functions of backfill placed between the rock and waste package need clearer definition and validation.The overall criterion to be used by federal agencies in designing a geologic waste-isolation system and in evaluating its nerformance has not yet been specified. As a guideline, the panel selected an average annual dose of 10-4 sieverts to a maximally exposed individual at any future time, if the exposure is from expected events such as the slow dissolution of waste solids in wet-rock repositories and the groundwater transport of dissolved radionuclides to the biosphere. Risks from unexpected events such as human intrusion were not evaluated.Calculations were made of the long-term isolation and environmental releases for conceptual repositories in basalt, granite, salt, and tuff. The major contributors to geologic isolation are the slow dissolution of key radioelements as limited by solubility and by diffusion and convection in groundwater surrounding the waste solids, long water travel times from the waste to the environment, and sorption retardation in the media surrounding the repository. Dilution by surface water can reduce the individual radiation exposures that can result from the small fraction of the waste radioactivity that may ultimately reach the environment. Estimates of environmental releases and individual doses were made both for unreprocessed spent fuel and for reprocessing wastes.Accelerated dissolution of waste exposed to groundwater during the period of repository heating was also considered. Long-term environmental releases of radioactivity from some repositories were calculated to cause doses to maximally exposed individuals that are several orders of magnitude below the Individual dose criterion of 10-4 Sieverts per year. Other conceptual repositories were found to not meet the individual dose criterion, although these repositories could still meet the radioactivity release limits in the standard proposed by the Environmental Protection Agency.The technology for geologic waste disposal has advanced to the state of a preliminary technical plan, suitable for testing, verification, and for pllot-facility confirmation. The waste Isolation program needs a reliable prediction of long-term performance that will serve as a basis for final design, construction, licensing, and waste emplacement.


1983 ◽  
Vol 26 ◽  
Author(s):  
Paul L. Chambre' ◽  
Thomas H. Pigford

ABSTRACTThe rate of dissolution of low-solubility species from waste forms in a geologic repository can be calculated from a theoretical analysis of the time-dependent rate of mass transfer by diffusion and convection Into the groundwater surrounding the waste, assuming a concentration at the waste-form surface eanal to the solubility of the radioelement. The analytical solutions for time-dependent mass transfer are reduced to asymptotic steady-state approximations valid over specified ranges of repository conditions. The predicted steady-state dissolution rates are considerably below those observed in laboratory leaching experiments with borosilicate glass and with other waste forms, indicating that the solid-liquid chemical reaction rates measured in the laboratory experiments are greater than the rates of diffusive-convective mass transfer in the concentration boundary layer surrounding the waste form in a geologic repository. It is shown that the time to reach steady-state dissolution can be as short as a few years, if convective mass transfer in the concentration boundary layer is important, to many thousands of years, If mass transfer is mainly by diffusion in the groundwater. The steady-state mass transfer rate can be Increased, and the time to reach steady state decreased, by sufficiently short half lives of the dissolving species. The theory has been extended to Include the effect of backfill on the steady-state mass transfer from the waste-form surface into moving groundwater.The mass-transfer theory has been extended to include the effect of time-dependent solubilities, diffusion coefficients, and retardation coefficients, which provides a means of calculating the time-dependent dissolution of lowsolubility species from waste exDosed to groundwater during the Period of repository heating. The effects of timetemperature transient dissolution on far-field concentrations and cumulative release are calculated.The transient and steady-state diffusion of radionuclides through a finite backfill layer separating a finite waste solid and porous rock has been analyzed, Including the effects of radioactive decay. Previous backfill analyses have neglected radioactive decay and have assumed an infinite amount of backfill. The results show that the break-through time and rate of radionuclide release depend on properties of the backfill and surrounding rock and on the waste form dimensions.Laboratory tests have been designed to validate these theoretical analyses of diffusive-convective mass transfer with solubility-limit boundary conditions. Preliminary tests are now underway at the Battelle Northwest Laboratory.Peak far-field concentrations of more soluble radionuclides such as cesium-135, with suitably long radionuclide transport times and sufficiently large axial dispersion, are shown to he insensitive to dissolution rate. Equivalent phenomena occur in fracture-flow radionuclide transport.


Author(s):  
T. J. Headley

Oxide phases having the hollandite structure have been identified in multiphase ceramic waste forms being developed for radioactive waste disposal. High resolution studies of phases in the waste forms described in Ref. [2] were initiated to examine them for fine scale structural differences compared to natural mineral analogs. Two hollandites were studied: a (Ba,Cs,K)-titan-ate with minor elements in solution that is produced in the waste forms, and a synthesized BaAl2Ti6O16 phase containing ∼ 4.7 wt% Cs2O. Both materials were consolidated by hot pressing at temperatures above 1100°C. Samples for high resolution microscopy were prepared both by ion-milling (7kV argon ions) and by crushing and dispersing the fragments on holey carbon substrates. The high resolution studies were performed in a JEM 200CX/SEG operating at 200kV.


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