Zirconium and Rubidium Solubility in Aluminoborosilicate Glasses for Radioactive Waste Immobilization

V. E. Eremyashev; Еремяшев В. Е.; G. G. Korinevskaya; Кориневская Г. Г.; M. A. Rassomakhin; Рассомахин М. А.; D. E. Zhivulin; Живулин Д. Е.

doi:10.31857/S0002337X2309004X

Zirconium and Rubidium Solubility in Aluminoborosilicate Glasses for Radioactive Waste Immobilization

Authors: Eremyashev V.E.¹, Korinevskaya G.G.¹^,2, Rassomakhin M.A.¹, Zhivulin D.E.²
Affiliations:
1. South Ural Federal Research Center of Mineralogy and Geoecology, Ural Branch, Russian Academy of Sciences
2. South Ural State University
Issue: Vol 59, No 9 (2023)
Pages: 1035-1042
Section: Articles
URL: https://ogarev-online.ru/0002-337X/article/view/249396
DOI: https://doi.org/10.31857/S0002337X2309004X
EDN: https://elibrary.ru/HXFQMM
ID: 249396

Cite item

Full Text

Open Access
Restricted Access

Access granted
Restricted Access

Subscription Access

Abstract
About the authors
References
Supplementary files
Statistics

Abstract

In search of novel waste form materials for vitrifying high-level radioactive waste with various compositions and improving the way in which they are used, we have prepared and investigated waste form materials in the Na2O–Rb2O–SrO(Ba,Ca)–B2O3–SiO2–Al2O3–ZrO2 system. Using electron microscopy, X-ray diffraction, and infrared spectroscopy characterization of samples prepared by rapid cooling of melts containing 3.6–4.5 mol % rubidium, we have demonstrated the formation of a homogeneous glassy material, determined the solubility limit of zirconium in the glass, and identified uniformly distributed baddeleyite crystals, which indicate that the starting melt contained excess zirconium. In samples containing 6.7–8.5 mol % rubidium, we observed the formation of a less homogeneous material with considerable amounts of crystalline zirconium- and rubidium-containing phases. Analysis of the data obtained has made it possible to optimize the percentages of zirconium and rubidium in the composition of radioactive waste in the case of its immobilization via vitrification with the use of waste form materials of the system studied here.

Keywords

radioactive waste, immobilization, aluminoborosilicate glass, rubidium, zirconium, structure

References

Caurant D., Loiseau P., Majérus O., Aubin-Chevaldonnet V., Bardez I., Quintas A. Glasses, Glass-Ceramics and Ceramics for Immobilization of Highly Radioactive Nuclear Wastes. N. Y.: Nova Science, 2009. 445 p.
Donald I.W. Waste Immobilization in Glass and Ceramic Based Hosts: Radioactive, Toxic and Hazardous Wastes. N. Y.: Wiley, 2010. 507 p. https://doi.org/10.1002/9781444319354
Ojovan M.I., Lee W.E., Kalmykov S.N. An Introduction to Nuclear Waste Immobilisation, 3rd ed. Amsterdam: Elsevier, 2019. P. 1–7. https://doi.org/10.1016/B978-0-08-102702-8.00001-7
Singh B.K., Hafeez M.A., Kim H., Hong S., Kang J., Um W. Inorganic Waste Forms for Efficient Immobilization of Radionuclides // ACS ES&T Eng. 2021. V. 1. № 8. P. 1149–1170. https://doi.org/10.1021/acsestengg.1c00184
Quintas A., Caurant D., Majerus O., Loiseau P., Charpentier T., Dussossoy J.-L. ZrO2 Addition in Soda-Lime Aluminoborosilicate Glasses Containing Rare Earths: Impact on the Network Structure // J. Alloys Compd. 2017. V. 714. P. 47–62. https://doi.org/10.1016/j.jallcom.2017.04.182
Vienna J.D., Collins E.D., Crum J.V., Ebert W.L., Frank S.M., Garn T.G., Gombert D., Jones R., Jubin R.T., Maio V., Marra J.C., Maty J., Nenoff T.M., Riley B.J., Sevigny G.J., Soelberg N., Strachan D., Thallapally P.K., Westsik J.H., Jr. Closed Fuel Cycle Waste Treatment Strategy, FCRD-MRWFD-2015-000674. PNNL-24114. Richland: Pacific Northwest National Laboratory, 2015. https://www.pnnl.gov/main/ publications/external/technical_reports/PNNL-24114.pdf
Lu X. et al. Effect of ZrO2 on the Structure and Properties of Soda-Lime Silicate Glasses from Molecular Dynamics Simulations // J. Non-Cryst. Solids. 2018. V. 491. P. 141–150. https://doi.org/10.1016/j.jnoncrysol.2018.04.013
Chen H., Marcial J., Ahmadzadeh M., Patil D., McCloy J.S. Partitioning of Rare Earths in Multiphase Nuclear Waste Glass-Ceramics // Int. J. Appl. Glass Sci. 2020. V. 11. P. 660–675. https://doi.org/10.1111/ijag.15726
Keshavarzi A., Russel C. The Effect of TiO2 and ZrO2 Addition on the Crystallization of Ce3+ Doped Yttrium Aluminium Garnet from Glasses in the System Y2O3/Al2O3/SiO2/AlF3 // Mater. Chem. Phys. 2012. V. 132. № 2. P. 278–83. https://doi.org/10.1016/j.matchemphys.2011.11.012
Guo Y., Liu C., Wang J., Ruan J., Li X., Han J., Xie J. Effect of ZrO2 Crystallization on Ion Exchange Properties in Aluminosilicate Glass // J. Eur. Ceram. Soc. 2020. V. 40. № 5. P. 2179–2184. https://doi.org/10.1016/j.jeurceramsoc.2020.01.001
Eremyashev V.E., Zherebtsov D.A., Osipova L.M., Danilina E.I. Thermal Study of Melting, Transition and Crystallization of Rubidium and Caesium Borosilicate Glasses // Ceram. Int. 2016. V. 42. P. 18368–18372. https://doi.org/10.1016/j.ceramint.2016.08.169
Еремяшев В.Е., Мазур А.С., Толстой П.М., Осипова Л.М. Исследование особенностей структуры рубидиевых боросиликатных стекол методом ЯМР-спектроскопии // Неорган. материалы. 2019. Т. 55. № 5. С. 538–543. https://doi.org/10.1134/S0020168519050054
Eremyashev V.E., Zherebtsov D.A., Brazhnikov M.P., Zainullina R.T., Danilina E.I. Cerium Influence on the Thermal Properties and Structure of High-Alkaline Borosilicate Glasses // J. Therm. Anal. Calorim. 2020. V. 139. № 2. P. 991–997.
Arima M., Edgar A.D. Stability of Wadeite (Zr2K4Si6O18) under Upper Mantle Conditions: Petrological Implications // Contr. Mineral. Petrol. 1980. V. 72. № 2. P. 191–195. https://doi.org/10.1007/bf00399479
Fewox C.S., Kirumakki S.R., Clearfield A. Structural and Mechanistic Investigation of Rubidium Ion Exchange in Potassium Zirconium Trisilicate // Chem. Mater. 2007. V. 19. № 3. P. 384–392. https://doi.org/10.1021/cm061835x
Lafuente B., Downs R.T., Yang H., Stone N. The Power of Databases: the RRUFF Project // Highlights in Mineralogical Crystallography / Eds. Armbruster T., Danisi R.M. Berlin: Gruyter, 2015. P. 1–30. http://rruff.info
Kyono A., Kimata M. Refinement of the Crystal Structure of a Synthetic Non-Stoichiometric Rb-Feldspar // Miner. Mag. 2001. V. 65. № 4. P. 523–531. https://doi.org/10.1180/002646101750377542
Nakamoto K. Infrared and Raman Spectra of Inorganic and Coordination Compounds // Handbook of Vibrational Spectroscopy. N. Y.: Wiley, 1986. 484 p. https://doi.org/10.1002/0470027320.s4104
Еремяшев В.Е., Осипов А.А., Осипова Л.М. Изучение влияния замещения катиона натрия катионами щелочноземельных металлов на структуру боросиликатных стекол // Стекло и керамика. 2011. № 7. С. 3–7. https://doi.org/10.1007/s10717-011-9353-5
Wan J., Cheng J., Lu P. The Coordination State of B and Al of Borosilicate Glass by IR Spectra // J. Wuhan Univ. Technol. Mater. 2008. V. 23. P. 419–421. https://doi.org/10.1007/s11595-007-3419-9