An international initiative on long-term behavior of high-level nuclear waste glass
Sandia National Laboratories1, Argonne National Laboratory2, University of Bonn3, National Nuclear Laboratory4, Kyushu University5, Japan Atomic Energy Agency6, Pacific Northwest National Laboratory7, Savannah River National Laboratory8, Pennsylvania State University9, Oak Ridge National Laboratory10, Amec Foster Wheeler11, Lawrence Berkeley National Laboratory12
TL;DR: A review of the state of the art in glass corrosion science can be found in this paper, where the authors briefly review the radioactive waste vitrification programs of the six participant nations and summarize the current state of glass corrosion research.
About: This article is published in Materials Today.The article was published on 2013-06-01 and is currently open access. It has received 401 citations till now. The article focuses on the topics: Radioactive waste.
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TL;DR: The low corrosion rate resulting from the formation of this stable passivating layer enables the objective of durability to be met, while progress in the fundamental understanding of corrosion unlocks the potential for optimizing the design of nuclear glass-geological disposal.
Abstract: Silicate glasses are durable materials, but are they sufficiently durable to confine highly radioactive wastes for hundreds of thousands years? Addressing this question requires a thorough understanding of the mechanisms underpinning aqueous corrosion of these materials. Here we show that in silica-saturated solution, a model glass of nuclear interest corrodes but at a rate that dramatically drops as a passivating layer forms. Water ingress into the glass, leading to the congruent release of mobile elements (B, Na and Ca), is followed by in situ repolymerization of the silicate network. This material is at equilibrium with pore and bulk solutions, and acts as a molecular sieve with a cutoff below 1 nm. The low corrosion rate resulting from the formation of this stable passivating layer enables the objective of durability to be met, while progress in the fundamental understanding of corrosion unlocks the potential for optimizing the design of nuclear glass-geological disposal
221 citations
Cites background from "An international initiative on long..."
...(1) The water mobility and reactivity within the alteration layer are lower than in the bulk solution....
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TL;DR: In this article, the authors summarized the current state of understanding of surface reactions, transport properties, and ion exchange along with the near-field materials and alteration products influences on solution chemistry and glass reaction rates.
Abstract: Chemical durability is not a single material property that can be uniquely measured. Instead it is the response to a host of coupled material and environmental processes whose rates are estimated by a combination of theory, experiment, and modeling. High-level nuclear waste (HLW) glass is perhaps the most studied of any material yet there remain significant technical gaps regarding their chemical durability. The phenomena affecting the long-term performance of HLW glasses in their disposal environment include surface reactions, transport properties to and from the reacting glass surface, and ion exchange between the solid glass and the surrounding solution and alteration products. The rates of these processes are strongly influenced and are coupled through the solution chemistry, which is in turn influenced by the reacting glass and also by reaction with the near-field materials and precipitation of alteration products. Therefore, those processes must be understood sufficiently well to estimate or bound the performance of HLW glass in its disposal environment over geologic time-scales. This article summarizes the current state of understanding of surface reactions, transport properties, and ion exchange along with the near-field materials and alteration products influences on solution chemistry and glass reaction rates. Also summarized are the remaining technicalmore » gaps along with recommended approaches to fill those technical gaps.« less
206 citations
TL;DR: In this paper, a cationic crystalline coordination polymer SBN was used to trap ReO4-incorporated phase (SBR) of anionic radioactive contaminant of great concern.
Abstract: We report one of the most efficient scavenger materials, a cationic crystalline coordination polymer SBN for trapping ReO4–, a surrogate for 99TcO4–, as an anionic radioactive contaminant of great concern. The uptake capacity for ReO4– reaches 786 mg/g, a value noticeably higher than the state of art anion-exchange resins and other inorganic or hybrid anion sorbents. Once being captured, ReO4– is greatly immobilized, as almost no ReO4– can be eluted using large excess of nitrate, carbonate, and phosphate anions. The processes are featured by a complete and irreversible single-crystal to single-crystal structural transformation from SBN to the ReO4–-incorporated phase (SBR). The coordination environments of NO3– and ReO4– probed by single-crystal structures clearly unravel the underlying mechanism, where each ReO4– in SBR binds to multiple Ag+ sites forming strong Ag–O–Re bonds, and to 4,4′-bipyridine through a dense hydrogen bond network. These structural insights lead to a significant difference in solub...
171 citations
TL;DR: In this paper, International Simple Glass (ISG) was altered at 90°C in a solution initially saturated with respect to amorphous 29SiO2, and the pH was raised to 11.5 after 209d by the addition of KOH.
165 citations
03 May 2018
TL;DR: In this article, the authors compare and contrast the mechanisms of environmental degradation of glass, crystalline ceramics, and metals, with the goal of identifying commonalities that can seed synergistic activities and advance the current knowledge in each area.
Abstract: All materials can suffer from environmental degradation; the rate and extent of degradation depend on the details of the material composition and structure as well as the environment. The corrosion of silicate glasses, crystalline ceramics, and metals, particularly as related to nuclear waste forms, has received a lot of attention. The corrosion phenomena and mechanisms of these materials are different, but also have many similarities. This review compares and contrasts the mechanisms of environmental degradation of glass, crystalline ceramics, and metals, with the goal of identifying commonalities that can seed synergistic activities and advance the current knowledge in each area.
164 citations
References
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01 Jan 1979
TL;DR: The Symposium on the Scientific Basis for Nuclear Waste Manage- ment was held in the fall of 1979 in Boston, Massachusetts and was one of a number of symposia included in the Annual Meeting of the Materials Research Society as mentioned in this paper.
Abstract: The Symposium on the Scientific Basis for Nuclear Waste Manage- ment was held in the fall of 1979 in Boston, Massachusetts and was one of a number of symposia included in the Annual Meeting of the Materials Research Society. The thrust of this annual Symposium is unique in the area of waste management. Recognizing that this is an area of great complexity which requires contributions from scien- tists with many different backgrounds some of which are not normally associated with nuclear energy, the Materials Research Society pro- vides a forum for discussions of a wide range of materials behavior and transport phenomena. As can be seen from the list of references in each paper, the authors draw heavily on contributions associated with professional societies in addition to the Materials Research Society, and this annual meeting encourages the cross-fertilization between disciplines that are essential to an adequate treatment of the problems associated with nuclear waste management. The proceed- ings of the first Symposium that was held in 1978 was designated as Volume 1 in this series. The third Symposium is scheduled for 1980. The scope of the 1979 Symposium was guided by the Steering Committee: R. L. Schwoebel, Sandia Laboratories, USA (Chairman) W. Carbiener, Battelle Memorial Institute, Columbus, USA D. Ferguson, Oak Ridge National Laboratory, USA W. Heimerl, DWK, Mol, Belgium W. Lutze, Hahn Meitner Institut, Berlin, W. Germany J. D. Mather, Institute of Geological Sciences, Harwell, UK G. Oertel, Department of Energy, USA R.
1,877 citations
TL;DR: In this article, the relative importance of the above reactions on glass degradation as a function of solution pH and composition, temperature and stress level was evaluated for silica, alkali silicate, and alkali boro- and aluminosilicate glasses.
Abstract: Dissolution, selective leaching, and stress-corrosion cracking are all processes which can degrade the performance of silica and silicate glasses exposed to aqueous environments. Reactions which corrode glass in water include hydration, hydrolysis and condensation, and ion-exchange processes. Techniques such as solid-state nuclear magnetic resonance, Raman and Fourier transform infrared spectroscopies, pH stat titrations and elemental depth profiling have been used to establish the relative importance of the above reactions on glass degradation as a function of solution pH and composition, temperature and stress level. This paper reviews results obtained for silica, alkali silicate, and alkali boro- and aluminosilicate glasses. For most glasses, the rate at which water enters the glass structure controls the kinetics of the other glass-water reactions, explaining the corrosion characteristics of different glass compositions.
523 citations
TL;DR: A new mechanism and impact of morphological transformations in the alteration layer on the leaching kinetics is demonstrated and a direct correlation between structure and reactivity is revealed by coupling the results of several structure-sensitive experiments with numerical simulations at mesoscopic scale.
Abstract: The remarkable chemical durability of silicate glass makes it suitable for a wide range of applications. The slowdown of the aqueous glass corrosion kinetics that is frequently observed at long time is generally attributed to chemical affinity effects (saturation of the solution with respect to silica). Here, we demonstrate a new mechanism and highlight the impact of morphological transformations in the alteration layer on the leaching kinetics. A direct correlation between structure and reactivity is revealed by coupling the results of several structure-sensitive experiments with numerical simulations at mesoscopic scale. The sharp drop in the corrosion rate is shown to arise from densification of the outer layers of the alteration film, leading to pore closure. The presence of insoluble elements in the glass can inhibit the film restructuring responsible for this effect. This mechanism may be more broadly applicable to silicate minerals.
401 citations
TL;DR: In this paper, experimental data on the interdiffusion of hydrogen and alkali ions in glass were examined using a concentration-dependent inter-diffusion coefficient, taking into account surface dissolution.
Abstract: Experimental data on the interdiffusion of hydrogen and alkali ions in glass are examined using a concentration-dependent interdiffusion coefficient, taking into account surface dissolution. The comparisons between calculated and experimental concentration profiles and diffusion coefficients are more satisfactory than for a concentration-independent diffusion coefficient, and support the use of the interdiffusion coefficient.
352 citations
TL;DR: In this article, the authors summarized the state of knowledge concerning aqueous alteration of R7T7-type nuclear containment glasses, represented mainly by the inactive reference glass designated SON68, and proposed a new mechanistic model known as GRAAL (glass reactivity with allowance for the alteration layer).
311 citations