Crystal Chemistry of Natural Zirconolite: Implications for High-Level Waste Incorporation in Synroc

1997 ◽  
Vol 506 ◽  
Author(s):  
Reto Gierpé ◽  
C. Terry Williams ◽  
Gregory R. Lumpkin
Keyword(s):  
Statistical Study ◽  
Alpha Decay ◽  
High Level Waste ◽  
Rock Types ◽  
Naturally Occurring ◽  
Geological Conditions ◽  
Wide Range ◽  
Alteration Processes ◽  
High Level Nuclear Waste ◽  
High Level

ABSTRACTZirconolite, ideally CaZrTi2O7, is a relatively rare mineral crystallizing at different geological conditions and in a wide range of generally SiO2-poor rock types. Synthetic zirconolite is one of two major actinide (ACT) host phases in SYNROC, a very promising option for the disposal of high-level nuclear waste (HLW). The available samples of naturally occurring zirconolite cover an extensive range in ACT content, age and host rock type, and thus offer an ideal opportunity to study the relationships between alpha-decay doses, radiation damage, and geochemical alteration processes [1]. In this paper, we present results obtained from a statistical study of nearly 300 chemical analyses of natural zirconolite [2].

The Salton Sea Geothermal Field as a Natural Analog for the Near-Field in a Salt High-Level Nuclear Waste Repository

1984 ◽  
Vol 44 ◽  
Author(s):  
Wilfred A. Elders ◽  
Judith B. Moody
Keyword(s):  
Nuclear Waste ◽  
Near Field ◽  
Geothermal Field ◽  
Salton Sea ◽  
High Level Waste ◽  
Nuclear Waste Repository ◽  
Natural Analog ◽  
Naturally Occurring ◽  
Wide Range ◽  
High Level

AbstractThe Salton Sea Geothermal Field (SSGF), on the delta of the Colorado River in southern California, is being studied as a natural analog for the near-field environment of proposed nuclear waste repositories in salt. A combination of mineralogical and geochemical methods is being employed to develop a three dimensional picture of temperature, salinity, lithology, mineralogy, and chemistry of reactions between the reservoir rocks and the hot brines. Our aim is to obtain quantitative data on mineral stabilities and on mobilities of the naturally occurring radionuclides of concern in Commercial High-Level Waste (CHLW). These data will be used to validate the EQ3/6 geochemical code under development to model the salt near-field repository behavior.Maximum temperatures encountered in wells in the SSGF equal or exceed peak temperatures expected in a salt repository. Brines produced from these wells have major element chemistry similar to brines from candidate salt sites. Relative to the rocks, these brines are enriched in Na, Mn, Zn, Sr, Ra and Po, depleted in Ba, Si, Mg, Ti, and Al, and strongly depleted in U and Th. However the unaltered rocks contain only about 2–3 ppm of U and 4–12 ppm of Th, largely in detrital epidotes and zircons. Samples of hydrothermally altered rocks from a wide range of temperature and salinity show rather similar uniform low concentrations of these elements, even when authigenic illite, chlorite, epidote and feldspar are present. These observations suggest that U and Th are relatively immobile in these hot brines. However Ra, Po, Cs and Sr are relatively mobile. Work is continuing to document naturally occurring radionuclide partitioning between SSGF minerals and brine over a range of temperature, salinity, and lithology.

Neptunium(V) Sorption Behavior on Clinoptilolite, Quartz and Montmorillonite

1995 ◽  
Vol 412 ◽  
Author(s):  
F. P. Bertetti ◽  
R. T. Pabalan ◽  
D. R. Turner ◽  
M. G. Almendarez
Keyword(s):  
Nir Spectroscopy ◽  
Electrolyte Solutions ◽  
Yucca Mountain ◽  
Sorption Behavior ◽  
Surface Loading ◽  
Wide Range ◽  
High Level Nuclear Waste ◽  
Ph Range ◽  
High Level ◽  
Carbonate Complexes

AbstractPerformance assessment models have identified 237Np as a radionuclide of concern in meeting release limits established for the geologic disposal of high-level nuclear waste at the proposed repository at Yucca Mountain, Nevada. In this study, quartz, clinoptilolite, and montmorillonite, which are minerals representative of phases that occur both in the rock matrix and as fracture coatings at Yucca Mountain, were reacted with 237Np-bearing solutions to characterize the sorption behavior of Np(V) on these minerals.Batch experiments were conducted over a wide range of conditions in which pH of solution, surface loading, sorbent surface area, initial concentration of Np(V), and partial pressure of CO2 were varied. Initial Np(V) concentrations were between 1 × 10-7 and 1- 10-6 M in electrolyte solutions of 0.1 or 0.01 M NaNO3. The oxidation state of Np in solution was verified with NIR spectroscopy and by solvent extraction. Prior to the start of experiments, minerals were pretreated to eliminate impurities, and the clinoptilolite and montmorillonite were converted to Na-form by ion exchange with NaCI solutions.Results indicate that, for all three minerals, Np(V) sorption begins at pH values coincident with the start of hydrolysis in solution (-7). For solutions undersaturated with respect to atmospheric CO2, sorption increases continuously with increasing pH. Under equilibrium with atmospheric CO2, Np(V) sorption is important in the pH range (7–9.5) where NpO2(OH)°(aq) is significant, whereas sorption is inhibited at higher pH where neptunyl carbonate complexes are the predominant species.

The Use of Repassivation Potential in Predicting The Performance of High-Level Nuclear Waste Container Materials

1994 ◽  
Vol 353 ◽  
Author(s):  
Narasi Sridhar ◽  
Darrell Dunn ◽  
Gustavo Cragnolino
Keyword(s):  
Field Tests ◽  
Localized Corrosion ◽  
High Level Waste ◽  
Repassivation Potential ◽  
Waste Container ◽  
Highly Sensitive ◽  
Plant Equipment ◽  
Robust Parameter ◽  
High Level Nuclear Waste ◽  
High Level

AbstractLocalized corrosion in aqueous environments forms an important bounding condition for the performance assessment of high-level waste (HLW) container materials. A predictive methodology using repassivation potential is examined in this paper. It is shown, based on long-term (continuing for over 11 months) testing of alloy 825, that repassivation potential of deep pits or crevices is a conservative and robust parameter for the prediction of localized corrosion. In contrast, initiation potentials measured by short-term tests are non-conservative and highly sensitive to several surface and environmental factors. Corrosion data from various field tests and plant equipment performance are analyzed in terms of the applicability of repassivation potential. The applicability of repassivation potential for predicting the occurrence of stress corrosion cracking (SCC) and intergranular corrosion in chloride containing environments is also examined.

An Approach to Analysis of High Level waste Container Performance in an Unsaturated Repository Environment

1993 ◽  
Vol 333 ◽  
Author(s):  
John C. Walton ◽  
Narasi Sridhar ◽  
Gustavo Cragnolino ◽  
Tony Torng ◽  
Prasad Nair
Keyword(s):  
Dominant Role ◽  
Near Field ◽  
Temperature Fields ◽  
Localized Corrosion ◽  
High Level Waste ◽  
Quantitative Methodology ◽  
Waste Container ◽  
Wide Range ◽  
Engineered Barrier ◽  
High Level

ABSTRACTOne of the requirements for the performance of waste packages prescribed in 10CFR 60.113 is that the high level waste must be “substantially completely” contained for a minimum period of 300 to 1000 years. During this period, the radiation and thermal conditions in the engineered barrier system and the near-field environment are dominated by fission product decay. In the present U.S design of the engineered barrier system, the outer container plays a dominant role in maintaining radionuclide containment. A quantitative methodology for analyzing the performance of the container is described in this paper. This methodology enables prediction of the evolution of the waste package environment in terms of temperature fields, stability of liquid water on the container surface, and concentration of aggressive ions such as chloride. The initiation and propagation of localized corrosion is determined by the corrosion potential of the container material and critical potentials for localized corrosion. The coiTOsion potential is estimated from the kinetics of the anodic and cathodic reactions including oxygen diffusion through scale layers formed on the container surface. The methodology described is applicable to a wide range of metals, alloys and environmental conditions.

Methodologies for Predicting the Performance of Ni-Cr-Mo Alloys Proposed for High Level Nuclear Waste Containers

1999 ◽  
Vol 556 ◽  
Author(s):  
D. S. Dunn ◽  
G. A. Cragnolino ◽  
N. Sridhar
Keyword(s):  
Nuclear Waste ◽  
Current Density ◽  
Localized Corrosion ◽  
Passive Current Density ◽  
Aqueous Corrosion ◽  
Wide Range ◽  
Anionic Species ◽  
High Level Nuclear Waste ◽  
High Level ◽  
Passive Current

AbstractFor the geologic disposal of the high level nuclear waste (HLW), aqueous corrosion is considered to be the most important factor in the long-term performance of containers, which are the main components of the engineered barrier subsystem. Container life, in turn, is important to the overall performance of the repository system. The proposed container designs and materials have evolved to include multiple barriers and highly corrosion resistant Ni-Cr-Mo alloys, such as Alloys 625 and C-22. Calculations of container life require knowledge of the initiation time and growth rate of localized corrosion. In the absence of localized corrosion, the rate of general or uniform dissolution, given by the passive current density of these materials, is needed. The onset of localized corrosion may be predicted by using the repassivation and corrosion potentials of the candidate container materials in the range of expected repository environments. In initial corrosion tests, chloride was identified as the most detrimental anionic species to the performance of Ni-Cr-Mo alloys. Repassivation potential measurements for Alloys 825, 625, and C-22, conducted over a wide range of chloride concentrations and temperatures, are reported. In addition, steady state passive current density, which will determine the container lifetime in the absence of localized corrosion, was measured for Alloy C-22 under various environmental conditions.

Nepheline Crystallization in High-Alumina High-Level Waste Glass

2015 ◽  
Vol 1744 ◽  
pp. 85-91 ◽  
Author(s):  
José Marcial ◽  
John McCloy ◽  
Owen Neill
Keyword(s):  
Nuclear Waste ◽  
Waste Glass ◽  
High Alumina ◽  
High Level Waste ◽  
Interfacial Conditions ◽  
Waste Vitrification ◽  
Cooling Schedules ◽  
High Level Nuclear Waste ◽  
High Level ◽  
Glass Compositions

ABSTRACTThe understanding of the crystallization of aluminosilicate phases in nuclear waste glasses is a major challenge for nuclear waste vitrification. Robust studies on the compositional dependence of nepheline formation have focused on large compositional spaces with hundreds of glass compositions. However, there are clear benefits to obtaining complete descriptions of the conditions under which crystallization occurs for specific glasses, adding to the understanding of nucleation and growth kinetics and interfacial conditions. The focus of this work was the investigation of the microstructure and composition of one simulant high-level nuclear waste glass crystallized under isothermal and continuous cooling schedules. It was observed that conditions of low undercooling, nepheline was the most abundant aluminosilicate phase. Further undercooling led to the formation of additional phases such as calcium phosphate. Nepheline composition was independent of thermal history.

scholarly journals Transporting and Storing High-Level Nuclear Waste in the U.S.—Insights from a Mathematical Model

2019 ◽  
Vol 9 (12) ◽  
pp. 2437 ◽  
Author(s):  
Sebastian Wegel ◽  
Victoria Czempinski ◽  
Pao-Yu Oei ◽  
Ben Wealer
Keyword(s):  
Nuclear Waste ◽  
The United States ◽  
Nuclear Industry ◽  
High Level Waste ◽  
Geological Repository ◽  
High Level Nuclear Waste ◽  
High Level ◽  
Interim Storage ◽  
Storage Facilities

The nuclear industry in the United States of America has accumulated about 70,000 metric tons of high-level nuclear waste over the past decades; at present, this waste is temporarily stored close to the nuclear power plants. The industry and the Department of Energy are now facing two related challenges: (i) will a permanent geological repository, e.g., Yucca Mountain, become available in the future, and if yes, when?; (ii) should the high-level waste be transported to interim storage facilities in the meantime, which may be safer and more cost economic? This paper presents a mathematical transportation model that evaluates the economic challenges and costs associated with different scenarios regarding the opening of a long-term geological repository. The model results suggest that any further delay in opening a long-term storage increases cost and consolidated interim storage facilities should be built now. We show that Yucca Mountain’s capacity is insufficient and additional storage is necessary. A sensitivity analysis for the reprocessing of high-level waste finds this uneconomic in all cases. This paper thus emphasizes the urgency of dealing with the high-level nuclear waste and informs the debate between the nuclear industry and policymakers on the basis of objective data and quantitative analysis.

Disposal of high-level nuclear wastes: a geological perspective

1985 ◽  
Vol 49 (351) ◽  
pp. 159-176 ◽  
Author(s):  
A. E. Ringwood
Keyword(s):  
Elevated Temperatures ◽  
Great Majority ◽  
Nuclear Industry ◽  
High Level Waste ◽  
Public Confidence ◽  
Wide Range ◽  
Close Relatives ◽  
High Level ◽  
Drill Holes

AbstractMost countries intend to dispose of their high-level radioactive wastes by converting them into a solidified wasteform which is to be buried within the earth. SYNROC is a titanate ceramic wasteform which has been designed for this purpose on the basis of geochemical principles. It comprises essentially rutile TiO2, ‘hollandite’ Ba(Al,Ti)Ti6O16, zirconolite CaZrTi2O7, and perovskite CaTiO3. The latter three phases have the capacity to accept the great majority of radioactive elements occurring in high-level wastes into their crystal lattice sites. These minerals (or their close relatives) also occur in nature, where they have demonstrated their capacity to survive for many millions of years in a wide range of geological environments. The properties of SYNROC and the crystal chemistry of its constituent minerals are reviewed in some detail and current formulations of SYNROC are summarized. A notable property of SYNROC it its extremely high resistance to leaching by groundwaters, particularly above 100°C. In addition, it can be shown that the capacity of SYNROC minerals to immobilize high-level waste elements is not markedly impaired by high levels of radiation damage. Current investigations are focused on developing a satisfactory production technology for SYNROC and progress towards this objective is described. The high leach resistance of SYNROC at elevated temperatures increases the range of geological environments in which the waste may be finally interred; in particular, SYNROC is well adapted for disposal in deep drill-holes, both in continental and marine environments. The fact that SYNROC is comprised of minerals which have demonstrated long-term geological stability is significant in establishing public confidence in the ability of the nuclear industry to immobilize high-level wastes for the very long periods required.

Corrosion Model Validation in High Level Nuclear Waste Package Research

1992 ◽  
Vol 294 ◽  
Author(s):  
M. B. Mcneil ◽  
J.B. Moody
Keyword(s):  
Site Specific ◽  
Waste Package ◽  
Naturally Occurring ◽  
Widespread Acceptance ◽  
Natural Analogues ◽  
High Level Nuclear Waste ◽  
Mineral Alteration ◽  
High Level ◽  
Performance Validation

ABSTRACTThe strategies for waste package (WP) performance validation will be based on site specific geologic and hydrogeochemical information plus models which can be used to predict potential WP lifetimes. The development and application of such models will include the evaluation of natural analogues (NA). These analogues are needed to resolve issues related to the validation of models. Natural analogues have not had extensive use or widespread acceptance in the area of waste package failure prediction. This lack of acceptance is due to the anticipated choice of alloys for waste package containers. Few of these alloys are similar to naturally occurring metals, and the proposed HLW repositories are in general in geologic settings not very similar to those in which naturally occurring metals are generally found.Natural and archaeological analogues can be used, however, in analysis of possible waste package failures as a means of testing proposed models for failure. In fact, the analogues are the only available mechanisms for testing models of long-term waste package behavior. A strategy is outlined for incorporating natural and archaeological analogue studies into waste package research, and examples are discussed. The natural/archaeological analogues approach which appears most promising is to use archaeological and mineral samples to develop an understanding of the identities and rates of the mineral alteration reactions at or near the surface of the package, improving present capability for estmating the lifetimes of metallic waste package containers.

The Kinetics of Spinel Crystallization from a High-Level Waste Glass

1996 ◽  
Vol 465 ◽  
Author(s):  
J. G. Reynolds ◽  
P. Hrma
Keyword(s):  
Volume Fraction ◽  
Treatment Time ◽  
Waste Glass ◽  
High Level Waste ◽  
Avrami Equation ◽  
Kinetic Coefficients ◽  
High Level Nuclear Waste ◽  
Isothermal Heat Treatments ◽  
High Level ◽  
Kinetics Of

ABSTRACTThe kinetics of spinel crystallization from a molten high-iron simulated high-level nuclear waste glass was studied using isothermal heat treatments. Optical microscopy with image analysis was used to measure volume fraction of spinel as a function of heat treatment time and temperature. The Johnson-Mehl-Avrami equation was fitted to data to determine kinetic coefficients for spinel crystallization. The liquidus temperature and Avrami number are TL = 1337K and n = 1.5.

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