A Flow Model for the Kinetics of Dissolution of Nuclear Waste Forms; A Comparison of Borosilicate Glass, Synroc and High-Silica Glass

1981 ◽  
Vol 11 ◽  
Author(s):  
Pedro B. Macedo ◽  
Aaron Barkatt ◽  
Joseoph H. Simmons

A model has been developed to predict the long-term leach or release rates of various waste-form materials under repository conditions.

Author(s):  
Martin W. A. Stewart ◽  
Sam A. Moricca ◽  
Tina Eddowes ◽  
Yingjie Zhang ◽  
Eric R. Vance ◽  
...  

ANSTO has developed a combination of tailored nuclear waste form chemistries coupled with the use of flexible hot-isostatic pressing processing technology to enable the successful incorporation of problematic nuclear wastes into dense, durable monoliths. This combined package also enables the design of waste forms with waste loadings well in excess of those achievable via baseline melting routes using borosilicate glass, as hot-isostatic pressing is not constrained by factors such as glass viscosity, crystallisation and electrical conductivity. In this paper we will discuss some of our experiences with problematic wastes, namely plutonium wastes, sludges and HLW such as the Idaho calcines.


1981 ◽  
Vol 6 ◽  
Author(s):  
Clyde J. M. Northrup ◽  
George W. Arnold ◽  
Thomas J. Headley

ABSTRACTThe first observations of physical and chemical changes induced by lead implantation damage and leaching are reported for two proposed U.S. nuclear waste forms (PNL 76–68 borosilicate glass and Sandia titanate ceramics) for commercial wastes. To simulate the effects of recoil nucleii due to alpha decay, the materials were implanted with lead ions at equivalent doses up to approximately 1 × 1019 a decays/cm3 . In the titanate waste form, the zirconolite, perovskite, hollandite, and rutile phases all exhibited a mottled appearance in the transmission electron microscope (TEM) typical of defect clusters in radiation damaged, crystalline solids. One titanate phase containing uranium was found by TEM to be amorphous after implantation at the highest dose. No enhanced leaching (deionized water, room temperature, 24 hours) of the irradiated titanate waste form, including the amorphous phase, was detected by TEM, but Rutherford backscattering (RBS) suggested a loss of cesium and calcium after 21 hours of leaching. The RBS spectra also indicated enhanced leaching from the PNL 76–68 borosilicate glass after implantation with lead ions, in general agreement with the observations of Dran, et al. [6,7] on other irradiated materials. Elastic recoil detection spectroscopy (ERD), used to profile hydrogen after leaching, showed penetration of the hydrogen to several thousand angstroms for both the implanted and unimplanted materials. These basic studies identified techniques to follow the changes that occur on implantation and leaching of complex amorphous and crystalline waste forms. These studies were not designed to produce comparisons between waste forms of gross leach rates.


2018 ◽  
Vol 47 (30) ◽  
pp. 10229-10239 ◽  
Author(s):  
Wayne W. Lukens ◽  
Sarah A. Saslow

The fission product, 99Tc, presents significant challenges to the long-term disposal of nuclear waste due to its long half-life, high fission yield, and to the environmental mobility of pertechnetate (TcO4−), the stable Tc species in aerobic environments.


1986 ◽  
Vol 84 ◽  
Author(s):  
Rodney C. Ewing ◽  
Michael J. Jercinovic

AbstractOne of the unique and scientifically most difficult aspects of nuclear waste isolation is the extrapolation ofshot-term laboratory data (hours to years) to the long time periods (103-105 years) required by regulatory agencies for performance assessment. The direct verification of these extrapolations is not possible, but methods must be developed to demonstrate compliance with government regulations and to satisfy the lay public that there is a demonstrable and reasonable basis for accepting the long-term extrapolations. Natural analogues of both the repository environment (e.g. radionuclide migration at Oklo) and nuclear waste form behavior (e.g. alteration of basaltic glasses and radiation damage in minerals) have been used to demonstrate the long-term behavior of large scale geologic systems and, on a smaller scale, waste form durability. This paper reviews the use of natural analogues to predict the long-term behavior of nuclear waste form glasses. Particular emphasis is placed on the inherent limitations of any conclusions that are based on “proof” by analogy. An example -- corrosion of borosilicate glass -- is discussed in detail with specific attention to the proper and successful use of natural analogues (basaltic glass) in understanding the long-term corrosion behavior of borosilicate glass.


1983 ◽  
Vol 26 ◽  
Author(s):  
M. Yasser Khalil ◽  
William B. White

ABSTRACTThe immobilization of 99Tc in both ceramic and borosilicate glass waste forms and the mechanism of dissolution of technetium from these waste forms are complicated by the range of technetium valence states. Metallic Tc,ionic Tc4+ oxides, and volatile molecular species containing Tc7+ all occur within the stability field of water. Tc4+ will substitute readily for Ti4+ in titanatebased ceramics in such phases as perovskite (CaTiO3) and spinel (Mg2TiO4). Tc4+ can be homogeneously distributed in borosilicate glass by re-melting the glass under closed system conditions to prevent the re-oxidation of technetium. The dissolution of technetium from both glass and ceramic waste forms follow similar kinetic behavior although the dissolution rate from the titanate is two orders of magnitude lower. Dissolution under highly reducing conditions is too slow to measure on the time scale of the experiments.


2019 ◽  
Vol 515 ◽  
pp. 227-237 ◽  
Author(s):  
James J. Neeway ◽  
R. Matthew Asmussen ◽  
Erin M. McElroy ◽  
Jacob A. Peterson ◽  
Brian J. Riley ◽  
...  

1986 ◽  
Vol 73 (2) ◽  
pp. 199-209 ◽  
Author(s):  
Pedro B. Macedo ◽  
Aaron Barkatt ◽  
Barbara C. Gibson ◽  
Charles J. Montrose

1992 ◽  
Vol 294 ◽  
Author(s):  
Rodney C. Ewing

ABSTRACTNatural materials may be used to advantage in the evaluation of the long-term performance of nuclear waste forms. Three case studies are presented: (I) radiation effects in ceramic waste forms; (II) corrosion products of U02 under oxic conditions; (III) corrosion rate of nuclear waste glasses. For each case, a natural phase which is structurally and chemically analogous to the waste form is identified and used to evaluate the long-term behavior of a nuclear waste form. Short-term experimental results are compared to the observations made of analogous natural phases. The three case studies illustrate that results may range between providing fundamental data needed for the long-term evaluation of a waste form to only providing qualitative data of limited use. Although in the most rigorous view the long-term behaviour of a phase cannot be predicted, the correspondence between short-term experimental results and observations made of natural phases provides confidence in the “predicted” behavior of the waste form. The strength of this approach rests with the degree to which a mechanistic understanding of the phenomenon is attained.


Author(s):  
Carol M. Jantzen

The long radioactive lifetime of the fission products in nuclear wastes requires that the materials be isolated from the biosphere for periods of 103 to 105 years. One method of accomplishing this is to consolidate the waste into a chemically stable solid form and to contain this within a multiple barrier canister which can be transported to a geologically stable repository for long-term storage. A number of candidate solid waste forms are being assessed to determine their suitability for incorporating various nuclear waste compositions and they include borosilicate glass (the current reference form), ceramics, high silica glasses, and cement.


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