Formation of Iron Phosphate Based Glass-ceramics for Nuclear Waste Immobilization by Microwave Sintering

Abstract

Iron phosphate based glass-ceramics with deliberately added Ce as an active nuclide simulant were prepared by microwave sintering. The sintering characteristics, including phases and structural evolution, and chemical durability were investigated. XRD showed that NaZr₂(PO₄)₃ and FePO₄ became the main crystalline phases of glass-ceramics with increasing sintering temperature. SEM revealed the glass-ceramics compactness increased first and then decreased as sintering temperature increased. Raman spectrum showed that, as sintering temperature increased, the network structure of glass-ceramics changed from mainly containing orthophosphate and pyrophosphate to a single orthophosphate. After immersion for 28 days, LR_Na, LR_Zr and LR_Ce of the glass-ceramics prepared at 1 000 °C were as low as 3.64×10⁻⁵, 0.25×10⁻⁹ and 5.70×10⁻⁹ g/m²/d respectively. The results indicate that iron phosphate based glass-ceramics can be prepared by rapid microwave sintering of glass powders and there is a potential of employing such microwave sintering technique in processing of glass-ceramics nuclear waste form.

Keywords

microwave sintering / iron phosphate / nuclear waste / glass-ceramics / chemical durability

References

[1] Weber W J, Navrotsky A, Stefanovsky S, et al.. Materials Science of High-level Nuclear Waste Immobilization[J]. MRS Bulletin, 2009, 34: 46-53

[2] Ojovan M I, Lee W E, Kalmykov S N, et al.. An Introduction to Nuclear Waste Immobilisation Second, 2019, UK, Elsevier167185[M]

[3] Bohre A, Avasthi K, Vladimir I, et al.. Vitreous and Crystalline Phosphate High Level Waste Matrices: Present Status and Future Challenges[J]. Journal of Industrial and Engineering Chemistry, 2017, 50: 1-14

[4] Donald I W, Metcalfe B L, Taylor R J, et al.. The Immobilization of High Level Radioactive Wastes Using Ceramics and Glasses[J]. Journal of Materials Science, 1997, 32: 5 851-5 887

[5] Gin S, Abdelouas A, Criscenti L J. An International Initiative on Long-term Behavior of High-level Nuclear Waste Glass[J]. Materials Today, 2014, 16: 243-248

[6] Yano K H, Mao K S, Wharry J P, et al.. Investing in a Permanent and Sustainable Nuclear Waste Disposal Solution[J]. Progress in Nuclear Energy, 2018, 108: 474-479

[7] Harrison M T. Vitrification of High Level Waste in the UK[J]. Procedia Materials Science, 2014, 7: 10-15

[8] Ojovan M I. Handbook of Advanced Radioactive Waste Conditioning Technologies, 2011, UK, Elsevier158236 M]

[9] Ramkumar J, Chandramouleeswaran S, Sudarsan V, et al.. Barium Borosilicate Glass as a Matrix for the Uptake of Dyes[J]. Journal of Hazardous Materials, 2009, 172: 457-464

[10] Kidari A, Dussossoy J L, Brackx E, et al.. Lanthanum and Neodymium Solubility in Simplified SiO₂–B₂O₃–Na₂O–Al₂O₃–CaO High Level Waste Glass[J]. Journal of the American Ceramic Society, 2012, 95: 2 537-2 544

[11] Caurant D, Majerus O, Loiseau P, et al.. Crystallization of Neodymium-rich Phases in Silicate Glasses Developed for Nuclear Waste Immobilization[J]. Journal of Nuclear Materials, 2006, 354: 143-162

[12] Stefanovsky S V, Stefanovsky O I, Danilov S S, et al.. Phosphate-based Glasses and Glass Ceramics for Immobilization of Lanthanides and Actinides[J]. Ceramics International, 2019, 45: 9 331-9 338

[13] McCarthy G J, White W B, Pfoertsch D E. Synthesis of Nuclear Waste Monazites, Ideal Actinide Hosts for Geologic Disposal[J]. Materials Research Bulletin, 1978, 13: 1 239-1 245

[14] Bingham P A, Hand R J, Forder S D. Doping of Iron Phosphate Glasses with Al₂O₃, SiO₂ or B₂O₃ for Improved Thermal Stability[J]. Materials Research Bulletin, 2006, 41: 1 622-1 630

[15] Bingham P A, Yang G, Hand R J, et al.. Boron Environments and Irradiation Stability of Iron Borophosphate Glasses Analysed by EELS[J]. Solid State Sciences, 2008, 10: 1 194-1 199

[16] Donald I W, Metcalfe B L. Thermal Properties and Crystallization Kinetics of a Sodium Aluminophosphate Based Glass[J]. Journal of Non-crystalline Solids, 2004, 348: 118-122

[17] Takebe H, Harada T, Kuwabara M. Effect of B₂O₃ Addition on the Thermal Properties and Density of Barium Phosphate Glasses[J]. Journal of Non-crystalline Solids, 2006, 352: 709-713

[18] Yao H, Xu X, Zhang R. Effect of Ti and Ce Microalloy on Microstructure and Properties of Al-Si-Cu-Zr-Sr Cast Aluminum Alloy[J]. Journal of Wuhan University of Technology-Mater Sci. Ed., 2023, 38.4: 897-902

[19] Caurant D, Loiseau P, Majerus O, et al.. Glasses, Glass-ceramics and Ceramics for Immobilization of Highly Radioactive Nuclear Wastes, 2007, Firt, Hauppauge, Nova Science162255[M]

[20] Zhou Z, He F, Shi M, et al.. Effect of Na2O Content on the Structure and Properties of Glass-ceramics Prepared by Spodumene[J]. Journal of Wuhan University of Technology-Mater. Sci. Ed., 2022, 37(5): 794-800

[21] Zhang Y, Zhang Z, Thorogood G, et al.. Pyrochlore Based Glass-ceramics for the Immobilization of Actinide-rich Nuclear Wastes: From Concept to Reality[J]. Journal of Nuclear Materials, 2013, 432: 545-547

[22] Crum J, Maio V, McCloy J, et al.. Cold Crucible Induction Melter Studies for Making Glass Ceramic Waste Forms: A Feasibility Assessment[J]. Journal of Nuclear Materials, 2014, 444: 481-492

[23] Liu Q, Feng L, Sun Y, et al.. Effects of Phosphate Glass on Cs⁺ Immobilization in Geopolymer Glass-ceramics[J]. Ceramics International, 2023, 49(4): 6 545-6 553

[24] Fen L, Hexi T, Xiaoyan S, et al.. Immobilization of Uranium-contaminated Soil Into Glass Waste by Microwave Sintering: Experimental and Theoretical Study[J]. Journal of Non-Crystalline Solids, 2020, 556(1): 120 551

[25] Wang X, Ruan J M, Chen Q Y. Effects of Surfactants on the Microstructure of Porous Ceramic Scaffolds Fabricated by Foaming for Bone Tissue Engineering[J]. Materials Research Bulletin, 2009, 44: 1 275-1 279

[26] ASTM. Standard Test Methods for Determining Chemical Durability of Nuclear, Hazardous, and Mixed Waste Glasses and Multiphase Glass Ceramics: the Product Consistency Test (PCT), 2014[S]

[27] Kaushik C P, Mishra R K, Sengupta P, et al.. Barium Borosilicate Glass-a Potential Matrix for Immobilization of Sulfate Bearing High-level Radioactive Liquid Waste[J]. Journal of Nuclear Materials, 2006, 358: 129-138

[28] Liu J, Wang F, Liao Q, et al.. Synthesis and Characterization of Phosphate-based Glass-ceramics for Nuclear Waste Immobilization: Structure, Thermal Behavior, and Chemical Stability[J]. Journal of Nuclear Materials, 2019, 513: 251-259

[29] Zhang L, Brow R K. A Raman Study of Iron–phosphate Crystalline Compounds and Glasses[J]. Journal of the American Ceramic Society, 2011, 94: 3 123-3 130

[30] Ray C S, Fang X, Karabulut M, et al.. Effect of Melting Temperature and Time on Iron Valence and Crystallization of Iron Phosphate Glasses[J]. Journal of Non-Crystalline Solids, 1999, 249: 1-16

[31] Moguš-Milanković A, Šantić A, Reis ST, et al.. Mixed Ion–polaron Transport in Na₂O – PbO–Fe₂O₃–P₂O₅ Glasses[J]. Journal of Non-Crystalline Solids, 2004, 342: 97-109

[32] Shi M, Liang Y, Chai L, et al.. Raman and FTIR Spectra of Modified Iron Phosphate Glasses Containing Arsenic[J]. Journal of Molecular Structure, 2015, 1081: 389-394

[33] Kamali K, Ravindran T R, Ravi C. Comparative Raman Spectroscopic Study of Phase Stability and Anharmonic Effects in AZr₂(PO₄)₃ (A=K, Rb and Cs)[J]. Spectrochimica Acta Part A: Molecular and Biomolecular Spectroscopy, 2016, 155: 38-46

[34] Brow R K, Tallant D R, Myers S T, et al.. The Short-range Structure of Zinc Polyphosphate Glass[J]. Journal of Non-Crystalline Solids, 1995, 191: 45-55

[35] Baran E J, Botto I L, Nord A G. The Vibrational Spectrum and the Conformation of the P₂O_4–7 Anion in Fe₂P₂O₇[J]. Journal of Molecular Structure, 1986, 143: 151-154

[36] Liu J, Zhu Y, Wang F, et al.. Properties and Structural Features of Iron Sodium Phosphate Glasses Containing Neodymium oxide[J]. Journal of Non-Crystalline Solids, 2018, 500: 92-97

[37] Lewis M H. Glasses and Glass-ceramics, 2013, UK, Springer Science[M]

[38] Crawford C L, Marra J C, Bibler N E. Glass Fabrication and Product Consistency Testing of Lanthanide Borosilicate Glass for Plutonium Disposition[J]. Journal of Alloys and Compounds, 2007, 444: 569-579

[39] Martin C, Ribet I, Frugier P, et al.. Alteration Kinetics of the Glass-ceramic Zirconolite and Role of the Alteration Film–Comparison with the SON68 Glass[J]. Journal of Nuclear Materials, 2007, 366: 277-287

[40] Fabian M, Pinakidou F, Tolnai I, et al.. Lanthanide (Ce, Nd, Eu) Environments and Leaching Behavior in Borosilicate Glasses [J]. Scientific Reports, 2021, 11: 13 272

[41] Wang F, Wang Y, Liao Q, et al.. Immobilization of a Simulated HLW in Phosphate Based Glasses/glass-ceramics by Melt-quenching Process[J]. Journal of Non-Crystalline Solids, 2020, 545: 120 246

[42] Xianhe M, Zhigui Q, Xiaoning Y, et al.. Immobilization of Simulated Radioactive Soil Waste Containing Cerium by Self-propagating High-temperature Synthesis[J]. Journal of Nuclear Materials, 2013, 443(1–3428-431

[43] Kim M, Heo J. Vitusite Glass-ceramics Wasteforms for Immobilization of Lanthanide Wastes Generated by Pyro-processing[J]. Ceramics International, 2015, 41(46 132-6 136

[44] Wang Z, Zhao Z, Peng B, et al.. Investigation on the Mechanism of the Immobilization of CeO₂ by Using Cullet-based Glass (CBG)[J]. Annals of Nuclear Energy, 2019, 133: 209-215

RIGHTS & PERMISSIONS

Wuhan University of Technology and Springer-Verlag GmbH Germany, Part of Springer Nature