Nuclear Engineering and Technology

Korean Nuclear Society (한국원자력학회)
권호 표지
DOI QR코드

DOI QR Code

Immobilization of sodium-salt wastes containing simulated 137Cs by volcanic ash-based ceramics with different Si/Al molar ratios

  • Sun, Xiao-Wen (School of Materials Science and Engineering, Southwest Jiaotong University) ;
  • Liu, Li-Ke (School of Materials Science and Engineering, Southwest Jiaotong University) ;
  • Chen, Song (School of Materials Science and Engineering, Southwest Jiaotong University)
  • Received : 2021.03.08
  • Accepted : 2021.06.20
  • Published : 2021.12.25
Download PDF
⟨ Previous Next ⟩

Abstract

In this study, volcanic ash was used as raw material to prepare waste forms with different silicon/aluminum (Si/Al) molar ratios to immobilize sodium-salt waste (SSW) containing simulated 137Cs. Effects of Si/Al molar ratios (3:1 and 2:1) and sodium salts on sintering behavior of waste forms and immobilization mechanism of Cs+ were investigated. Results indicated that the main mineral phase of sintered waste-form matrixes was albite, and the formation of major phases was found to depend on Si/Al molar ratios. Si/Al molar ratio of 2 was favorable for the formation of pollucite, and the formation and crystallization of mineral phases were also decided based on physicochemical characteristics of sodium salts. Furthermore, product consistency test results indicated that the immobilization of Cs+ was related to Si/Al molar ratio, types of sodium salts, and glassy phase. Waste forms with Si/Al molar ratio of 2 exhibited better ability to immobilize Cs+, whereas the influence of sodium salts and glassy phases on the immobilization of SSW showed more complicated relationship. In waste forms with Si/Al molar ratio of 2, Cs+ leaching concentrations of samples containing Na2B4O7·10H2O and NaOH were low. Na2B4O7·10H2O easily transformed into liquid phase during sintering to consequently achieve low temperature liquid-phase sintering, which is beneficial to avoid the volatilization of Cs+ at high temperature. Results clearly reveal that waste forms with Si/Al molar ratio of 2 and containing Na2B4O7·10H2O show excellent immobilization of Cs+.

Keywords

Acknowledgement

This work was supported by the Sichuan Provincial Science and Technology Program Project (No. 21SYSX0170).

References

  1. Xu Kai, Review of international research progress on nuclear waste vitrification, Mater China 35 (7) (2016) 481-488.
  2. M.I. Ojovan, W.E. Lee, An Introduction to Nuclear Waste Immobilisation, Elsevier, Amsterdam, 2005, pp. 1-15.
  3. Y. Yokomori, K. Asazuki, N. Kamiya, et al., Final storage of radioactive cesium by pollucite hydrothermal synthesis, Sci. Rep. 4 (2014) 4195. https://doi.org/10.1038/srep04195
  4. M. Schneider, The world nuclear industry status report 2015, Bull. At. Sci. 68 (5) (2015) 8-22. https://doi.org/10.1177/0096340212459126
  5. Z. Jing, W. Hao, X. He, et al., A novel hydrothermal method to convert incineration ash into pollucite for the immobilization of a simulant radioactive cesium, J. Hazard Mater. 306 (2016) 220-229. https://doi.org/10.1016/j.jhazmat.2015.12.024
  6. M. Omerasevic, L. Matovic, J. Ruzic, et al., Safe trapping of cesium into pollucite structure by hot-pressing method, J. Nucl. Mater. 474 (2016) 35-44. https://doi.org/10.1016/j.jnucmat.2016.03.006
  7. K.L. Nash, G.J. Lumetta, Advanced Separation Techniques for Nuclear Fuel Reprocessing and Radioactive Waste Treatment, Woodhead Publishing Limited, Oxford Cambridge Philadelphia New Delhi, 2011, pp. 4-17.
  8. F. Register, Separations/Reprocessing. Nuclear Wastes: Technologies for Separations and Transmutation, 1996, pp. 35-47.
  9. Ning Shun Yan, Wang Xin Peng, Qing Zou, et al., Direct separation of minor actinides from high level liquid waste by me 2 -CA-BTP/SiO2-P adsorbent, Sci. Rep. 7 (1) (2017) 14679. https://doi.org/10.1038/s41598-017-14758-2
  10. Wu Jian Jiang, Several preparation methods of cesium metal, Xinjiang Youse Jinshu 5 (2012) 48-49.
  11. C. Kunzel, J.F. Cisneros, T.P. Neville, et al., Encapsulation of Cs/Sr contaminated clinoptilolite in geopolymers produced from metakaolin, J. Nucl. Mater. 466 (2015) 94-99. https://doi.org/10.1016/j.jnucmat.2015.07.034
  12. J.B. Pacesa, K.R. Ludwigb, Z.E. Petermana, et al., 234U/238U evidence for local recharge and patterns of ground-water flow in the vicinity of yucca mountain,Nevada,USA, Appl. Geochem. 17 (6) (2002).
  13. H. Fujiwara, H. Kuramochi, K. Nomura, et al., Behavior of radioactive cesium during incineration of radioactively contaminated wastes from decontamination activities in Fukushima, J. Environ. Radioact. 178-179 (nov) (2017) 290-296. https://doi.org/10.1016/j.jenvrad.2017.08.014
  14. A K T , A D P , B I J , et al. Radioactive waste management in Croatia - public opinion, legal framework, and policy. Energy Pol., 146.
  15. C.S.L.I. Yuxiang, Research Actualities on High-Level Waste Forms, Materials Review, 2005.
  16. C. Che, Y. Teng, Q. Gui, Research and application status of radioactive waste solidification, Mater. Rev. 20 (2) (2006) 94-97. https://doi.org/10.3321/j.issn:1005-023X.2006.02.025
  17. A. Monteiro, Schuller, S. Toplis, et al., Chemical and mineralogical modifications of simplified radioactive waste calcine during heat treatment, J. Nucl. Mater. 448 (1) (2014) 8-19. https://doi.org/10.1016/j.jnucmat.2014.01.012
  18. C.M. Jantzen, W.E. Lee, M.I. Ojovan, Radioactive waste conditioning, immobilization, and encapsulation processes and technologies: overview and advances, in: Radioactive Waste Management and Contaminated Site Clean-up: Processes, Technologies and International Experience, Woodhead Publishing, Cambridge, UK, 2013, pp. 6-10 (Chapter 6) in.
  19. J.H. Yang, H.S. Park, Y.Z. Cho, Immobilization of Cs-trapping ceramic filters within glass-ceramic waste forms, Ann. Nucl. Energy 110 (2017) 1121-1126. https://doi.org/10.1016/j.anucene.2017.08.051
  20. B.D. Williams, J.J. Neeway, M.M.V. Snyder, et al., Mineral assemblage transformation of a metakaolin-based waste form after geopolymer encapsulation, J. Nucl. Mater. (2016) 320-332.
  21. J. Yuan, P. He, X. Liang, et al., Thermal evolution of lithium ion substituted cesium-based geopolymer under high temperature treatment, Part I: effects of holding temperature, Ceram. Int. (2018), S0272884218304930.
  22. E. Ofer-Rozovsky, M.A. Haddad, G. Bar-Nes, et al., Cesium immobilization in nitrate-bearing metakaolin-based geopolymers, J. Nucl. Mater. 514 (2018) 247-254.
  23. J. Mon, Y. Deng, M. Flury, et al., Cesium incorporation and diffusion in cancrinite, sodalite, zeolite, and allophane, Microporous Mesoporous Mater. 86 (1-3) (2005) 277-286. https://doi.org/10.1016/j.micromeso.2005.07.030
  24. P. He, D. Jia, M. Wang, et al., Effect of cesium substitution on the thermal evolution and ceramics formation of potassium-based geopolymer, Ceram. Int. 36 (8) (2010) 2395-2400. https://doi.org/10.1016/j.ceramint.2010.07.015
  25. N. Meller, C. Hall, Hydroceramic Sealants for Geothermal Wells, 2004.
  26. D. Siemer, Hydroceramics, a "new" Cementitious Waste Form Material for U.S. Defense-type Reprocessing Waste, Materials Research Innovations, 2002.
  27. Y. Bao, M.W. Grutzeck, C.M. Jantzen, Preparation and properties of hydroceramic waste forms made with simulated hanford Low〢ctivity waste, J. Am. Ceram. Soc. 88 (12) (2005).
  28. K. Kyritsis, C. Hall, D.P. Bentz, et al., Relationship between engineering properties, mineralogy, and microstructure in cement-based hydroceramic materials cured at 200°-350℃, J. Am. Ceram. Soc. 92 (2009) 694-701. https://doi.org/10.1111/j.1551-2916.2008.02914.x
  29. Y. Bao, M.W. Grutzeck, Solidification of sodium bearing waste using hydroceramic and portland cement binders, Ceram. Trans. (2004) 168.
  30. J. Wang, J. Wang, Y. Zhang, et al., Properties of alkali-activated slag-fly ashmetakaolin hydroceramics for immobilizing of simulated sodium-bearing waste, Prog. Nucl. Engergy 93 (2016) 12-17. https://doi.org/10.1016/j.pnucene.2016.07.021
  31. J. Wang, J. Wang, Y. Huang, et al., Preparation of alkali-activated slag-fly ashmetakaolin hydroceramics for immobilizing simulated sodium-bearing waste, J. Am. Ceram. Soc. 98 (5) (2015) 1393-1399. https://doi.org/10.1111/jace.13489
  32. S. Fu, P. He, M. Wang, et al., Hydrothermal synthesis of pollucite from metakaolin-based geopolymer for hazardous wastes storage, J. Clean. Prod. 248 (Mar.1) (2020) 119240.1-119240.10.
  33. N.J. Hess, Espinosa, et al., Beta radiation effects in {sup 137Cs-substituted pollucite, J. Nucl. Mater. (2000) 281.
  34. L.H. Ortega, M.D. Kaminski, S.M. Mcdeavitt, Pollucite and feldspar formation in sintered bentonite for nuclear waste immobilization, Appl. Clay Sci. 50 (4) (2010) 594-599. https://doi.org/10.1016/j.clay.2010.10.003
  35. Z.H.A.O. Yu-long, L.I. Bao-jun, Z.H.O.U. Hui, et al., Immobizition of simulated cesium-137 waste in synroc, J. Nucl. Radiochem. (3) (2005) 152-157.
  36. You Jin-song, Ceramic Mechanism and Thermal Properties of Sodium and Lithium Substituted Cubic Cesium Leucite Compounds Using Geopolymer Method, Harbin Institute of Technology, 2015.
  37. Rui-fei Wang, Immobilization of Simulated Radionuclide 133Cs+ by Geopolymer, Harbin Institute of Technology, 2018, pp. 77-78.
  38. Zhen Xu, Preparation and Characterization of Glass Ceramics and Artificial Rock Soildified Body, Chengdu University of Technology, 2016.
  39. V.P.O. Solutions, W.C.O. Gases, D.O.P. Substances, et al., Perry's Chemical Engineers' Handbook, McGraw-Hill, 2013.
  40. H. Schultz, The Essential Structure and Properties of Glass, China Construction Industry Press, 1984.
  41. S. Chen, Z. Sun, D.G. Zhu, Mineral-phase evolution and sintering behavior of MO-SiO2-Al2O3-B2O3 (M = Ca, Ba) glass-ceramics by low-temperature liquid-phase sintering, Int. J. Minerals Metal. Mater. 25 (9) (2018) 1042-1054. https://doi.org/10.1007/s12613-018-1655-y
  42. D.N. Yoon, W.J. Huppmann, Grain growth and densification during liquid phase sintering of W-Ni, Acta 27 (4) (1979) 693-698.