Gamma irradiation-induced defects in borosilicate glasses for high-level radioactive waste immobilisation

Rautiyal, Prince; Gupta, Gaurav; Edge, Ruth; Leay, Laura; Daubney, Aaron; Patel, Maulik; Jones, Alan Hywel; Bingham, Paul A.

doi:10.1016/j.jnucmat.2020.152702

Cited by 27 publications

(23 citation statements)

References 100 publications

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“…The E opt values estimated were 3.71 (±0.05), 3.74 (±0.04), and 3.74 (±0.04) eV for the ISG, ISG‐1, and ISG‐2 samples, respectively. These values are found within the estimate by Rautiyal et al 43 . for borosilicate glasses of the Li 2 O‐Na 2 O‐B 2 O 3 ‐SiO 2 and Na 2 O‐BaO‐B 2 O 3 ‐SiO 2 type reported at 3.90 and 3.50 eV, respectively, studied also in the context of high‐level radioactive waste immobilization.…”

Section: Resultssupporting

confidence: 90%

Physico‐chemical properties of international simple glass (ISG) nuclear waste simulants: Luminescence baseline study

2022

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Borosilicate glass has been adopted internationally for the treatment of nuclear waste with the object of long‐term stabilization through vitrification. Aiming to facilitate experimental comparisons across laboratories, the six‐component international simple glass (ISG) was developed as benchmark. The original ISG produced by Mo‐SCI Corporation (Rolla, MO) was distributed and characterized for different physical properties thus serving as reference for further studies. Still, photoluminescence (PL) properties, which may be useful for scrutinizing radiation‐induced damage, have not been reported. Further, the original ISG contained significant iron impurities, which may present interference in various studies (e.g., optical). Consequently, two new ISG analogs lacking iron impurities (labeled ISG‐1 [closest composition to original ISG] and ISG‐2 [some MgO added at expense of CaO]) were synthesized by Corning Inc. (Corning, NY) (also doped with lanthanum for subsequent corrosion tests involving atom probe tomography), which remain to be fully characterized. Accordingly, this work was undertaken to perform a comprehensive study comparing the three ISG specimens. Various characterizations were then performed on the pristine glasses: X‐ray diffraction and vibrational spectroscopy (structural properties); static‐leach product consistency test (PCT, dissolution behavior); dilatometry and calorimetry measurements (thermal properties); and optical absorption with Tauc and Urbach plots analysis, followed by PL spectroscopy with decay kinetics assessment (optical properties). While the general structural features appeared similar among the glasses, the deconvolution of Raman spectra suggested a lower degree of connectivity in the silica network for ISG‐2. In addition, some differences were indicated from the PCT results and thermal properties assessed, which were discussed based on compositional variations. Further on, the optical properties were shown to be the most distinct. The optical absorption of the original ISG was characterized by Fe2+/Fe3+ impurities not detected for ISG‐1 and ISG‐2. The glasses all exhibited two main PL features (∼1.8 and 2.5 eV) with multiexponential decay behavior apparently of intrinsic origin. In addition, ISG‐1 and ISG‐2 showed a third high‐energy (∼3.4 eV) fast‐decaying contribution tentatively credited to tin impurities, which appeared most significantly for ISG‐1. The results are expected to serve as baseline for future studies simulating the effects of radioactive element decay.

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Section: Resultssupporting

confidence: 90%

Physico‐chemical properties of international simple glass (ISG) nuclear waste simulants: Luminescence baseline study

2022

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“…The possible reason is that the maximum of the absorbed dose in this work is two orders of magnitude lower than that in Ollier's work 14 . Rautiyal showed Raman spectra of borosilicate glasses with the absorbed dose of 1 × 10 6 Gy, in which no oxygen molecule peak appeared 54 …”

Section: Resultsmentioning

confidence: 62%

“…14 Rautiyal showed Raman spectra of borosilicate glasses with the absorbed dose of 1 × 10 6 Gy, in which no oxygen molecule peak appeared. 54 Besides the oxygen atoms that are left from the network of glass, those in the network of glass could be separated into two parts: BO and NBO. The XPS spectra could discriminate the difference between the BO and NBO.…”

Section: X-rays Photoelectron Spectroscopy (Xps) Spectramentioning

confidence: 99%

Structural changes on the surfaces of borosilicate glasses induced by gamma‐ray irradiation

Mao

Yang

et al. 2022

J Am Ceram Soc.

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Vitrification is a kind of glass that can solidify high‐level radioactive waste (HLW). As the basic material of vitrification, borosilicate glass was studied extensively. To keep HLW away from the biosphere, the tolerance of borosilicate glass to irradiation is important. In this work, various samples of borosilicate glass with different compositions were irradiated with gamma rays at ambient temperature to study their stability. The hardness, moduli, and microscopic changes on surfaces of the borosilicate glasses were measured at specific absorbed doses. Upon the gamma irradiation, the structural changes on surfaces of borosilicate glasses were identified, which were strongly influenced by the composition of borosilicate glasses. The results demonstrate that gamma irradiation, as well as beta irradiation, might strongly influence the properties of vitrification. The irradiation effects on vitrification induced by gamma irradiation should be paid more attention to than before.

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“…The complex network structure of borosilicate glasses has been under scrutiny for decades to account for important properties of nuclear-waste materials such as the solubilities of radioactive ions, − long-term chemical durability, ,− radiation damage, − and phase separation. , High-level radioactive waste (HLW) comprises more than 30 different oxides, many of which are radioactive, with half-lives ranging from a few days to millions of years . Aluminum is the third most abundant species in HLW from the Hanford Nuclear Site and can be a prominent component in HLW from other origins; hence, the extent of its incorporation into borosilicate glasses impacts the total waste-loading capacity.…”

Section: Introductionmentioning

confidence: 99%

Network Formation in Borosilicate Glasses with Aluminum or Gallium: Implications for Nepheline Crystallization

2021

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The evolution of the network connectivity of borosilicate glasses with the progressive addition of aluminum is analyzed using solid-state multinuclear magnetic resonance (NMR) spectroscopy to better understand the structural mechanism by which boron inhibits nepheline crystallization in nuclear-waste glasses. The [4]Al units exert a stronger influence on Na+ than do the [4]B units, resulting in the reorganization of tetrahedral to trigonal-planar boron ([4]B → [3]B) with increasing Al. The [3]B units preferably bond to [4]Al and interfere with the Si–Al ordering critical to nepheline formation, thereby inhibiting nucleation. Moreover, as Na+ charge compensates both [4]B and [4]Al units, the presence of anionic borate units confers a heterogeneous chemical environment about Na+ and prevents its transformation into a nepheline-like crystalline environment. The NMR results for aluminoborosilicate glasses are compared with those of their gallium analogues to assess the structural similarities of Al and Ga in silicate-based glasses. Gallium integrates into the borosilicate network as tetrahedral units similar to Al but is less effective in competing with [4]B for Na+, leading to higher [4]B ratios. The relative fractions of silicate Q3 and Q4 species are determined semiquantitatively using charge-balance constraints on 29Si NMR results, showing that the silicate speciation in high-Ga glasses is restricted to Q4 units, which may affect the properties relevant to nuclear-waste immobilization.

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Gamma irradiation-induced defects in borosilicate glasses for high-level radioactive waste immobilisation

Cited by 27 publications

References 100 publications

Physico‐chemical properties of international simple glass (ISG) nuclear waste simulants: Luminescence baseline study

Physico‐chemical properties of international simple glass (ISG) nuclear waste simulants: Luminescence baseline study

Structural changes on the surfaces of borosilicate glasses induced by gamma‐ray irradiation

Network Formation in Borosilicate Glasses with Aluminum or Gallium: Implications for Nepheline Crystallization

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