Leaching of borosilicate glasses. II. Model and Monte-Carlo simulations

Devreux, F.; Ledieu, A.; Barboux, P.; Minet, Y.

doi:10.1016/j.jnoncrysol.2004.06.007

Cited by 71 publications

(108 citation statements)

References 13 publications

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“…82 The MC simulations were performed in two phases: the dissolution and the condensation phase, 82,83 while more complex algorithms were adopted in more recent MC simulations. 84 In the dissolution phase, the surface grids were scanned and the soluble species such as sodium and boron were dissolved unconditionally while the silicon Q n species were dissolved based on the probability w n .…”

Section: First-principles-based Simulations Of Glass-water Interactionsmentioning

confidence: 99%

Atomistic computer simulations of water interactions and dissolution of inorganic glasses

Rimsza

2017

npj Mater Degrad

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Computer simulations at the atomistic scale play an increasing important role in understanding the structure features, and the structure-property relationships of glass and amorphous materials. In this paper, we reviewed atomistic simulation methods ranging from first principles calculations and ab initio molecular dynamics (AIMD) simulations, to classical molecular dynamics (MD), and meso-scale kinetic Monte Carlo (KMC) simulations and their applications to study the reactions and interactions of inorganic glasses with water and the dissolution behaviors of inorganic glasses. Particularly, the use of these simulation methods in understanding the reaction mechanisms of water with oxide glasses, water-glass interfaces, hydrated porous silica gels formation, the structure and properties of multicomponent glasses, and microstructure evolution are reviewed. The advantages and disadvantageous of these simulation methods are discussed and the current challenges and future direction of atomistic simulations in glass dissolution presented.npj Materials Degradation (2017) 1:16 ; doi:10.1038/s41529-017-0017-yThe corrosion or degradation of glasses in aqueous solutions are critical in a number of engineering and technological processes ranging from microelectronic packaging, glass reaction chambers, and the immobilization of nuclear waste materials, as well as in healthcare and biomedical fields such as dissolution of inhaled glass fibers and bioactive glasses for biomedical applications. In particular, immobilizing radioactive waste in borosilicate glasses is widely accepted as a preferred method to treat nuclear waste materials generated from civilian and military sources. This process, also known as vitrification, is a critical component of the cycle of nuclear energy to combat global environmental and energy challenges. Researchers from around the world have extensively invested in understanding glass corrosion in an effort to predict the long-term stability and release rate radionuclides to the environment during nuclear waste storage. 1,2Various mechanisms for glass corrosion have been proposed and despite intensive experimental investigations with advanced characterization techniques results are unclear. It is generally accepted that the corrosion of glass consists of a set of complex processes including hydration, hydrolysis, and ion-exchange that are coupled during glass dissolution. The initial stage is interdiffusion of proton or hydronium ions from the solution with sodium or other alkali ions in the glass.3 This is followed by the hydrophilic attack of water on the Si-O-Si or Si-O-Al linkages that lead to hydroxylation of the silicate glass network. The remaining hydrolyzed glass skeleton then undergoes condensation and repolymerization to form the hydrated nanoporous silica rich gel layer which can be protective, decreasing dissolution to a residual rate. [4][5][6] The morphology of the gel layer, such as thickness, pore structure, and chemical composition, depends on the original glass composition and the pH...

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Section: First-principles-based Simulations Of Glass-water Interactionsmentioning

confidence: 99%

Atomistic computer simulations of water interactions and dissolution of inorganic glasses

Rimsza

2017

npj Mater Degrad

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“…So, Si should prefer to dissolve from the outer surface of the gel, and experiments validate this [52]. Secondly, GM models consider the gel as a constant composition boundary, but more resent research found that the gel morphology is changing constantly during glass alteration, and even can close the "kinetic reaction path" [53,54,61,62]. Thirdly, the use of the factor f ret to describe the weight fraction of initially dissolved Si, which became incorporated into secondary alteration products or sorbed on the glass surface, appears to be an over simplification.…”

Section: A C C E P T E D Accepted Manuscriptmentioning

confidence: 96%

“…Thirdly, the use of the factor f ret to describe the weight fraction of initially dissolved Si, which became incorporated into secondary alteration products or sorbed on the glass surface, appears to be an over simplification. These two processes would have very different effect on the corrosion of glass -they both decrease the chemical affinity, but the weight fraction of Si sorbed on the glass surface can result in a densifying reaction and have significant effect on "kinetic reaction path [14,53,54,61,62].…”

Section: A C C E P T E D Accepted Manuscriptmentioning

confidence: 99%

“…In addition, this model emphasizes on Na、B、Si as they were the most familiar elements which can reveal the dissolution rate of borosilicate glass. Ledieu [61], Devreux [62] investigated leaching behaviour of borosilicate glasses. Their result showed that the leached fractions LF(B) and LF(Na) are low and nearly equal to LF(Si) for the glasses with boron (and sodium) oxide content less than 15 mol%.…”

Section: A C C E P T E D Accepted Manuscriptmentioning

confidence: 99%

“…steadystate concentration [61,62,74,75]. Take case 3 in section 4.2.1 as an example, according to equation (16), the evolution of Si concentration in solution can be divided into two stages, when C d (t) < C d ,:" * , C d (t) can be described as:…”

Section: Rules Of Key Elements Release From Glass During Leaching Timementioning

confidence: 99%

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A mechanistic model for long-term nuclear waste glass dissolution integrating chemical affinity and interfacial diffusion barrier

Jivkov

et al. 2017

Journal of Nuclear Materials

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Abstract:Understanding the alteration of nuclear waste glass in geological repository conditions is critical element of the analysis of repository retention function. Experimental observations of glass alterations provide a general agreement on the following regimes: inter-diffusion, hydrolysis process, rate drop, residual rate and, under very particular conditions, resumption of alteration. Of these, the mechanisms controlling the rate drop and the residual rate remain a subject of dispute. This paper offers a critical review of the two most competitive models related to these regimes: affinity-limited dissolution and diffusion barrier. The limitations of these models are highlighted by comparison of their predictions with available experimental evidence. Based on the comprehensive discussion of the existing models, a new mechanistic model is proposed as a combination of the chemical affinity and diffusion barrier concepts. It is demonstrated how the model can explain experimental phenomena and data, for which the existing models are shown to be not fully adequate.Key words: nuclear waste glasses, long-term dissolution, mechanisms, modelling IntroductionRadioactivity wastes are generated at all stages of the nuclear fuel cycle, including the decommissioning of nuclear facilities, as well as from military applications. Of particular concern for the storage/disposal of radioactivity wastes are those containing long-lived radionuclides [1].The current plan ( countries such as Belgium, Finland , Sweden , France etc.)for long-term management of such wastes is to store them in deep, stable and lowpermeable geological formations [2].The storage design is based on the so-called multi-barrier concept, where several barriers prevent for a period of time, or slow down the release and migration of radionuclides through the geosphere [3,4].Within this concept, hazardous nuclides are immobilized into solidified bodies. The wasteform selection is difficult, since durability is not the sole criterion [5]. Currently, vitrification is regarded as the best solution for immobilizing radionuclides. This technology has been progressively developed over the last half-century, has matured and has become industrially robust.Data collected to date suggest that glass waste forms offer the advantages that they can accommodate a wide range of waste streams, are resistant to radiation damage, and are relatively inert to both chemical and thermal perturbations [6].The use of natural and archeological analogues supported further the durability argument of glass as waste forms [7][8][9][10][11]. Except for the alumino-phosphate glass used in Russia, the borosilicate glass has been universally selected by all other nations [12].In order to make scientifically-underpinned safety cases, the long-term behaviour of glassy wasteforms requires further understanding and assessment. Half-lives of some radionuclides extend to millions of years, requiring isolation for geological periods, while the period of investigation possible in the field and the la...

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