Self-healing capacity of nuclear glass observed by NMR spectroscopy

Charpentier, Thibault; Martel, Laura; Mir, Anamul Haq; Somers, J.; Jégou, Christophe; Peuget, S.

doi:10.1038/srep25499

Cited by 43 publications

(56 citation statements)

References 35 publications

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“…The decrease of 8.9% in the proportion of BO 4 groups in the rapidly quenched glass is closer to the one observed in radioactive ISG doped with 244 Cm (7%), 12 than to the decrease induced in ISG by heavy-ions (Au) irradiation (13%). 13 Furthermore, whereas a change in aluminum coordination and depolymerization was observed for the irradiated glass, 12 no such changes were observed either for 244 Cm doped ISG 13 or for the quenched fibers in this study. These results therefore support the use of rapid quenching to mimic the effects of self-irradiation in nuclear glasses.…”

Section: Discussionmentioning

confidence: 69%

“…11 However, glasses submitted to external heavy-ion irradiation, simulating the effect of the recoil nuclei, show more significant effects than those seen in 244 Cm doped glasses. 12,13 This behavior was attributed to the local annealing induced by the alpha particle's loss of electronic energy that partially repairs the damages generated by the recoil nuclei. 14 Structural changes induced by self-irradiation could in particular affect the alteration behavior of glass matrices.…”

Section: Introductionmentioning

confidence: 99%

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Effect of thermally induced structural disorder on the chemical durability of International Simple Glass

et al. 2018

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While the influence of silicate oxide glass composition on its chemical durability is increasingly known, the contribution of structure only is less well understood, yet is crucial for an accurate description of aqueous alteration mechanisms. The effect of structural disorder can be investigated by varying the thermal history of the glass. Furthermore, the structural changes generated by selfirradiation in nuclear glasses can be compared with those induced by fast quenching. In the context of deep geological disposal of vitreous matrices, it is then challenging to address the structural impact on glass durability. Here, a borosilicate glass, the International Simple Glass, was fiberized to obtain a rapidly quenched sample. The quenching rate and fictive temperature were evaluated from in situ Raman and Brillouin spectroscopies. Multinuclear nuclear magnetic resonance was used to obtain insight into the effect of quenching on the pristine and altered glass structure. Higher bond angle distribution and lower mixing of alkalis were observed in the fast quenched glass. Some of AlO 4 groups are then Ca-compensated, while a part of BO 4 is transformed into BO 3 units. The structural modifications increase the hydrolysis of the silicate network occurring in the forward rate regime at 90°C by a factor of 1.4-1.8 depending on the pH value. Residual rate regime is similarly affected, more significantly at the beginning of the experiments conducted in silica saturated solutions. These findings prove that the reactivity of glass remains controlled by its structure under the various alteration regimes.

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Section: Discussionmentioning

confidence: 69%

Section: Introductionmentioning

confidence: 99%

Effect of thermally induced structural disorder on the chemical durability of International Simple Glass

et al. 2018

Self Cite

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“…Al K-edge could not be investigated as the lowest beamline energy available on MARS is around 3.5 keV, to be compared to the 1.5 kev absorption edge threshold for Al K-edge. Furthermore, a recent NMR study on the same glass [14] shows that there is no structural evolution around Al species between the damaged glass and the annealed one.…”

Section: Introductionmentioning

confidence: 95%

“…Apart from the measurements of macroscopic physical quantities, like density, hardness or mechanical properties [6], considering the radioactive nature of the samples, sparse experimental techniques are available to investigate the glass structure under self-irradiation condition such as vibrational Raman technique [7,8], X-Ray Fluorescence (XRF), X-ray Absorption Spectroscopy (XAS) [6,7,[9][10][11][12][13] and more recently Nuclear Magnetic Resonance (NMR) [14].…”

Section: Introductionmentioning

confidence: 99%

XANES analysis of a Cm-doped borosilicate glass under $$\alpha $$ α -self-irradiation effects

Bouty

Ramond²,

Solari

et al. 2016

J Mater Sci

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Industrial borosilicate glasses containing fission products and minor actinides can be subjected to structural damage caused mainly by a-self-irradiation effects. In this field of glasses under extreme conditions, we present an X-ray Absorption Near-Edge Structure investigation of two six-oxide borosilicate curium-doped glasses (based on the International Simplified Glass (ISG) composition). The first sample is an 8-year ISG damaged glass, which has already accumulated an a-decay dose greater than 6.10 18 a g À1 , a value corresponding to a damaged but stabilized structural state. The second sample results from annealing of the latter ISG damaged glass. Three species, Cm, Pu and Zr were probed at L 3 -edge, L 3 -edge and K-edge, respectively. From the experimental results, Cm and Pu species appear respectively in ?3 and ?4 oxidation states in both glasses. No Cm local environment changes are observed. In contrast, a small variation in Pu local environment appears between the damaged and annealed glasses, reflecting a possible coordination variation or Pu-Zr substitution. A more drastic effect appears for Zr local environment, where a sevenfold coordinated site grows over time under a-self-irradiation effects, at the expense of the initial major sixfold site of symmetry. Moreover, annealing the damaged glass does not permit to retrieve a similar structural state to the one of a just melted curium-doped ISG.

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“…1 International Simple Glass (ISG) is a simplified model composition for a collaborative study of dissolution/corrosion mechanism of highlevel waste (HLW) glasses. [2][3][4] ISG has been intensively researched recently with studies focusing on its dissolution behavior under different conditions, 3,[5][6][7][8][9][10][11][12] its surface quality, 13 radiation effect, [14][15][16][17][18] waste loading, 19 mechanical property, 20,21 and especially on the properties of its alteration layers using diverse techniques such as electron microprobe analysis, 22 Doppler broadening positron annihilation spectroscopy, 23 and atom probe tomography. 24 However, due to the lack of long-range periodicity, the structural study of glass materials exhibits many challenges.…”

Section: Introductionmentioning

confidence: 99%

Structural role of ZrO2 and its impact on properties of boroaluminosilicate nuclear waste glasses

Deng

Kerisit

et al. 2018

npj Mater Degrad

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Addition of zirconia (ZrO 2 ) to nuclear waste glasses, even in small amount, significantly affects physical properties such as chemical durability, density, viscosity, and glass transition temperature. Hence ZrO 2 plays an important role in the development of nuclear waste glass compositions. It was found recently that addition of zirconia decreases the initial dissolution rate but increases longterm dissolution by changing the protective properties such as porosity of alteration layers. In this study, the International Simple Glass (ISG) with different amounts of ZrO 2 /SiO 2 substitution was simulated using classical molecular dynamics (MD) simulations and recently developed composition-dependent potential sets. Local structural descriptors such as bond distances, bond angle distributions, and coordination numbers were systematically studied and compared with experimental values. Zr K-edge extended X-ray absorption fine structure spectra were also calculated and compared with experiment to resolve the local coordination environment around Zr. Medium-range structural information (e.g., Q n distribution, network connectivity, and ring-size distribution) showed that ZrO 2 /SiO 2 substitution increases the overall network connectivity and the amount of smaller sized rings, which will decrease the initial dissolution rate by strengthening the glass network and limiting water diffusivity. Finally, diffusion and dynamic properties of the ions were studied and discussed to develop a better understanding of the chemical durability of these glasses.

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Self-healing capacity of nuclear glass observed by NMR spectroscopy

Cited by 43 publications

References 35 publications

Effect of thermally induced structural disorder on the chemical durability of International Simple Glass

Effect of thermally induced structural disorder on the chemical durability of International Simple Glass

XANES analysis of a Cm-doped borosilicate glass under $$\alpha $$ α -self-irradiation effects

Structural role of ZrO2 and its impact on properties of boroaluminosilicate nuclear waste glasses

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