Self-propagating High-temperature Synthesis of Sm and Zr Co-doped Gd2Ti2O7 Pyrochlore Ceramics as Nuclear Waste Forms

Dayan Xie , Kuibao Zhang , Weiwei Li , Baozhu Luo , Haiyan Guo

Journal of Wuhan University of Technology Materials Science Edition ›› 2021, Vol. 36 ›› Issue (2) : 196 -202.

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Journal of Wuhan University of Technology Materials Science Edition ›› 2021, Vol. 36 ›› Issue (2) : 196 -202. DOI: 10.1007/s11595-021-2394-x
Advanced Materials

Self-propagating High-temperature Synthesis of Sm and Zr Co-doped Gd2Ti2O7 Pyrochlore Ceramics as Nuclear Waste Forms

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Abstract

We reported a rapid synthesis of Sm3+/Zr4+ co-doped Gd2Ti2O7 pyrochlore simulated nuclear wastes solidification by self-propagation plus quick pressing technique. With increment excess contents of Sm2O3 and ZrO2 from 0 to 10wt%, the phase composition of the products is a mixed phase of pyrochlore structure and defective fluorite structure by X-ray diffraction (XRD) analysis and Raman spectrum. In addition, the SEM results demonstrate the fracture surface and microstructure of Gd2Ti2O7-based pyrochlore. The densified pyrochlore waste form exhibits high bulk density of 5.56 g·cm−3 and vickers hardness of 11.20±0.2 GPa. The leaching tests show that the elemental leaching rates of Gd, Sm, and Cu after 42 days are 1.92×10−4, 1.51×10−4, and 3.90×10−3 g·m−2·d−1, respectively.

Keywords

SHS / pyrochlore / immobilization of nuclear wastes / excess

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Dayan Xie, Kuibao Zhang, Weiwei Li, Baozhu Luo, Haiyan Guo. Self-propagating High-temperature Synthesis of Sm and Zr Co-doped Gd2Ti2O7 Pyrochlore Ceramics as Nuclear Waste Forms. Journal of Wuhan University of Technology Materials Science Edition, 2021, 36(2): 196-202 DOI:10.1007/s11595-021-2394-x

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References

[1]

Ojovan MI, Lee WE. Immobilisation of Radioactive Wastes in Bitumen[J]. An Introduction to Nuclear Waste Immobilisation, 2005: 201–212

[2]

Fehrenbach L, Maurette M, Guichard F, et al. Paleocorrosion Studies in Deep Sea Sediments and the Geological Disposal of Nuclear Wastes[J]. Journal of Non-Crystalline Solids, 1984, 67(1–3): 287-303.

[3]

Bates EA, Salazar A, Driscoll MJ, et al. Plug Design for Deep Borehole Disposal of High-level Nuclear Waste[J]. Nuclear Technology, 2014, 188(3): 280-291.

[4]

Chapman N, Hooper A. The Disposal of Radioactive Wastes Under-ground[J]. Proceedings of the Geologists Association, 2012, 123(1): 46-63.

[5]

Huang W, Day DE, Ray CS, et al. Vitrification of High Chrome Oxide Nuclear Waste in Iron Phosphate Glasses[J]. Journal of Nuclear Materials, 2004, 327(1): 46-57.

[6]

Blair Thomas H. Full-scale in-can Melting for Vitrification of Nuclear Wastes[J]. Transactions of the American Entomological Society, 1978, 28(2): 267-273.

[7]

Donald IW, Metcalfe BL, Taylor R. The Immobilization of High Level Radioactive Wastes Using Ceramics and Glasses[J]. Journal of Materials Science, 1997, 32(22): 5 851-5 887.

[8]

Kikuchi M, Chino K, Nishi T, et al. Radioactive Waste Treatment Using Cement-glass Solidification Technique[J]. Journal of Nuclear Science Technology, 1992, 29: 1 026-1 032.

[9]

Luo S, Li L, Tang B, et al. Synroc Immobilization of High Level Waste (HLW) Bearing a High Content of Sodium[J]. Waste Management, 1998, 18(1): 55-59.

[10]

Fairhall G, Johnson G, Newland K. Conference on Materials and Nuclear Power[J]. The Institute of Materials, 1996: 197–204

[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(1–3): 143-162.

[12]

He ZS, Zhang KB, Peng L, et al. Self-propagating Plus Quick Pressing Synthesis and Characterizations of Gd2−xNdxTi1.3Zr0.7O7 (0⩽ x ⩽ 1.4) Pyrochlores[J]. Journal of Nuclear Materials, 2018, 504: 61-67.

[13]

Peng L, Zhang KB, He ZS, et al. Self-propagating High-temperature Synthesis of ZrO2 Incorporated Gd2Ti2O7 Pyrochlore[J]. Journal of Advance Ceramic, 2018, 7: 41-49.

[14]

Zhang KB, Wen G, Zhang HB, et al. Self-propagating High-temperature Synthesis of Y2Ti2O7 Pyrochlore and Its Aqueous Durability[J]. Journal of Nuclear Materials, 2015, 465: 1-5.

[15]

Campbell J, Hoenig C, Ryerson F, et al. Immobilization of High-level Defense Wastes in SYNROC: An Appraisal of Product Performance[J]. Presented at High Level Waste Tech Rev., 1981

[16]

Ringwood AE, Oversby VM, Kesson SE. Immobilization of High-level Nuclear Reactor Wastes in SYNROC: A Current Appraisal[J]. Nucl Chem Waste Manage, 1981, 2: 287-305.

[17]

Lian J, Helean KB, Kennedy BJ, et al. Effect of Structure and Thermodynamic Stability on the Response of Lanthanide Stannate Pyrochlores to Ion Beam Irradiation.[J]. Journal of Physical Chemistry B, 2006, 110(5): 2 343-2 350.

[18]

Wang J, Wang JX, Zhang YB, et al. Flux Synthesis and Chemical Stability of Nd and Ce Co-doped (Gd1−xNdx)2(Zr1−xCex)2O7 (0 ⩽ x ⩽ 1) Pyrochlore Ceramics for Nuclear Waste Forms[J]. Ceramic International, 2017, 43: 17 064-17 070.

[19]

Ewing RC, Weber WJ, FWC Jr. Radiation Effects in Nuclear Waste Forms for High-level Radioactive Waste[J]. Progress in Nuclear Energy, 1995, 29(2): 63-127.

[20]

Sickafus KE, Minervini L, Grimes RW, et al. Radiation Tolerance of Complex Oxides[J]. Science, 2000, 289: 748-751.

[21]

Weber WJ, Ewing RC, Angell CA, et al. Radiation Effects in Glasses Used for Immobilization of High-level Waste and Plutonium Disposition[J]. Journal of Materials Research, 1997, 12(08): 1 948-1 978.

[22]

Mao XH, Qin ZG, Yuan XN, et al. Immobilization of Simulated Radioactive Soil Waste Containing Cerium by Self-propagating High-temperature S ynthesis[J]. Journal of Nuclear Materials, 2013, 443: 428-431.

[23]

Zhang YJ, Li HJ, Moricca S. Pyrochlore-structured Titanate Ceramics for Immobilisation of Actinides: Hot Isostatic Pressing (HIPing) and Stainless Steel/Waste form Interactions[J]. Journal of Nuclear Materials, 2008, 377: 470-475.

[24]

Merzhanov AG. History and Recent Developments in SHS[J]. Ceramic International, 1995, 21: 371-379.

[25]

Glagovskii M, Kuprin AV, Pelevin LP, et al. Immobilization of High-level Wastes in Stable mineral-like Materials in a Self-propagating High-temperature Synthesis Regime[J]. Atomic Energy, 1999, 87(1): 514-518.

[26]

Muthuraman M, Dhas NA, Patil KC. Combustion Synthesis of Oxide Materials for Nuclear Waste Immobilization[J]. Bulletin of Materials Science, 1994, 17(6): 977-987.

[27]

Zhang KB, Yin D, Han PW, et al. Two-step Synthesis of Zirconolite-rich Ceramic Waste Matrice and Its Physicochemical Properties[J]. International Journal of Applied Ceramic Technology, 2018, 15(1): 171-178.

[28]

Zhang KB, Yin D, Lu XR, et al. Self-propagating High-temperature Synthesis, Phase Composition and Aqueous Durability of Nd-Al Bearing Zirconolite-rich Composites as Nuclear Waste Form[J]. Adv Appl Ceram, 2017, 117: 78-84.

[29]

Zhang KB, Yin D, Peng L, et al. Self-propagating Synthesis and CeO2 Immobilization of Zirconolite-rich Composites using CuO as the Oxidant[J]. Ceramics International, 2016, 43(1): 1 415-1 423.

[30]

Zhang KB, Yin D, Peng L, et al. Self-propagating Synthesis of Nd2O3-incorporated Zirconolite/Mo Composites and Their Aqueous Durability[J]. Journal of Nuclear Materials, 2017, 491: 177-182.

[31]

Zhang RZ, Hao JJ, Guo ZM. Synthesis of SrTiO3 for Immobilization of Simulated HLW by SHS[J]. Journal of University of Science & Technology Beijing, 2005, 12(004): 357-359.

[32]

Zhang RZ, Shi SJ, Zhang TP, et al. Strontium Titanate Immobilization of Simulated HLW by SHS[J]. Advanced Science Letters, 2012, 12(1): 381-384.

[33]

Zhang RZ, Zhao JH, Guo ZM. Synthesis of SrTiO3 by Double-SHS for Immobilization of High Level Radioactive Waste[J]. Chinese Journal of Rare Metals, 2009, 33(1): 66-70.

[34]

Peng L, Zhang KB, Yin D, et al. Self-propagating Synthesis, Mechanical Property and Aqueous Durability of Gd2Ti2O7 Pyrochlore[J]. Ceramics International, 2016, 42: 18 907-18 913.

[35]

Daniel JL, Mellinger GB, Barner JO. Reference and Testing Materials Available from the Materials Characterization Center[J]. Mrs Proceedings, 1984, 44: 723.

[36]

Helean KB, Begg BD, Navrotsky A, et al. Enthalpies of Formation of Gd2(Ti2−xZrx)O7 Pyrochlores[J]. MRS Proceedings, 2000, 663

[37]

Mori M, Tompsett GM, Sammes NM, et al. Compatibility of GdxTi2O7 Pyrochlores (1.72⩽x⩽2.0) as Electrolytes in High-temperature Solid Oxide Fuel Cells[J]. Solid State Ionics, 2003, 158(1): 79-90.

[38]

Lummen, Handayani IP, Donker M, et al. Phonon and Crystal Field Excitations in Geometrically Frustrated Rare Earth Titanates[J]. Physical review B, 2008, 77(21)

[39]

Sattonnay G, Moll S, Thome L, et al. Phase Transformations Induced by High Electronic Excitation in Ion-irradiated Gd2(ZrxTi1x)2O7 Pyrochlores[J]. Journal of Applied Physics, 2010, 108(10): 103 512-103 512.

[40]

Maczka M, Hanuza J, Hermanowicz K, et al. Temperature-dependent Raman Scattering Studies of the Geometrically Frustrated Pyrochlores Dy2Ti2O7, Gd2Ti2O7 and Er2Ti2O7[J]. Journal of Raman Spectroscopy, 2008, 39(4): 537-544.

[41]

Mączka M, Sanjuán ML, Fuentes AF, et al. Temperature-dependent Studies of the Geometrically Frustrated Pyrochlores Ho2Ti2O7 and Dy2Ti2O7[J]. Physical Review B, 2009, 79(21): 1 377-1 381.

[42]

Zhang FX, Manoun B, Saxena SK. Pressure-induced Order-disorder Transitions in Pyrochlore RE2Ti2O7 (RE=Y,Gd)[J]. Materials Letters, 2006, 60(21): 2 773-2 776.

[43]

Sanjuán ML, Guglieri C, DíazMoreno S, et al. Raman and X-ray Absorption Spectroscopy Study of the Phase Evolution Induced by Mechanical Milling and Thermal Treatments in R2Ti2O7 Pyrochlores[J]. Physical review B, 2011, 84: 104207.

[44]

Zhang Y, Stewart M, Li H, et al. Zirconolite-rich Titanate Ceramics for Immobilisation of Actinides-Waste form/HIP can Interactions and Chemical Durability[J]. Journal of Nuclear Materials, 2009, 395(1): 69-74.

[45]

Ojovan MI, Lee WE. Glassy Wasteforms for Nuclear Waste Immobilization[J]. Metallurgical and Materials Transactions A, 2011, 42: 837-851.

[46]

Ledieu A, Devreux F, Barboux P, et al. Leaching of Borosilicate Glasses. I. Experiments[J]. Journal of Non-Crystalline Solids, 2004, 343(1–3): 3-12.

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