Fe2O3对含铈钙钛矿玻璃陶瓷物相结构及化学稳定性的影响

摘要/Abstract

摘要： 本文以典型SiO₂-B₂O₃-CaO-Na₂O-TiO₂硼硅酸盐玻璃为基础玻璃,采用热处理析晶法制备含铈钙钛矿玻璃陶瓷固化体。通过DSC、XRD、FTIR、SEM-EDS、ICP等测试方法研究了不同Fe₂O₃含量对该固化体物相结构及化学稳定性的影响。结果表明,随着Fe₂O₃的掺入,CeO₂晶体衍射峰强度逐渐减弱,钙钛矿(CaTiO₃)晶粒分布的均匀程度呈先升高后降低的趋势,所有元素的归一化浸出率呈先降低后升高的趋势。当Fe₂O₃含量为6%(质量分数)时,CeO₂晶体消失,晶粒的分布最为均匀,所有元素的归一化浸出率最低。28 d后,所有样品中元素的归一化浸出率(g·m^-2·d^-1)均低于10^-3数量级,这表明所制备的玻璃陶瓷固化体具有优异的化学稳定性。本研究为采用钙钛矿玻璃陶瓷固化体处理高放核废液提供了理论支撑和实验指导。

关键词: Fe₂O₃, 钙钛矿, 氧化铈, 玻璃陶瓷, 物相结构, 化学稳定性

Abstract: In this paper, based on the typical SiO₂-B₂O₃-CaO-Na₂O-TiO₂ borosilicate glass, the cerium-containing perovskite glass-ceramic waste form was prepared by heat treatment crystallization method. The effect of different Fe₂O₃ content on the phase structure and chemical stability of the waste form was studied by DSC, XRD, FTIR, SEM-EDS and ICP. The results show that with the addition of Fe₂O₃, the diffraction peak intensity of CeO₂ crystal gradually decreases, the uniform of perovskite (CaTiO₃) grain distribution shows a trend of increasing first and then decreasing, and the normalized leaching rates of all elements show a trend of decreasing first and then increasing. When the content of Fe₂O₃ is 6% (mass fraction), the CeO₂ crystal disappears, the distribution of grains is the most uniform, and the normalized leaching rate of elements is the lowest. After 28 d, the normalized leaching rates (g·m^-2·d^-1) of elements in all samples are lower than the order of magnitude of 10^-3, indicating that the prepared glass-ceramic waste form has excellent chemical stability. The findings of this research offer theoretical support and experimental guidance for the study of perovskite glass-ceramics solidified high-level liquid waste.

Key words: Fe₂O₃, perovskite, cerium oxide, glass-ceramics, phase structure, chemical stability

中图分类号:

TQ171

蒲博洋, 廖其龙, 王辅, 古雨鑫, 胥有利, 竹含真. Fe₂O₃对含铈钙钛矿玻璃陶瓷物相结构及化学稳定性的影响[J]. 硅酸盐通报, 2024, 43(4): 1308-1317.

PU Boyang, LIAO Qilong, WANG Fu, GU Yuxin, XU Youli, ZHU Hanzhen. Effect of Fe₂O₃ on Phase Structure and Chemical Stability of Cerium-Containing Perovskite Glass-Ceramics[J]. BULLETIN OF THE CHINESE CERAMIC SOCIETY, 2024, 43(4): 1308-1317.

参考文献

[1] KUMAR A, KULRIYA P K, SHARMA S K, et al. Structural and compositional effects on the electronic excitation induced phase transformations in Gd₂Ti_2-yZr_yO₇ pyrochlore[J]. Journal of Nuclear Materials, 2020, 539: 152278.
[2] WU K M, WANG F, LIAO Q L, et al. Synthesis of pyrochlore-borosilicate glass-ceramics for immobilization of high-level nuclear waste[J]. Ceramics International, 2020, 46(5): 6085-6094.
[3] ZHANG Y J, MIR A H. A review of brannerite structured materials for nuclear waste management[J]. Journal of Nuclear Materials, 2023, 583: 154512.
[4] KONG L G, ZHANG Y J, KARATCHEVTSEVA I. Preparation of Y₂Ti₂O₇ pyrochlore glass-ceramics as potential waste forms for actinides: the effects of processing conditions[J]. Journal of Nuclear Materials, 2017, 494: 29-36.
[5] ZHU H Z, WANG F, LIAO Q L, et al. Structure features, crystallization kinetics and water resistance of borosilicate glasses doped with CeO₂[J]. Journal of Non-Crystalline Solids, 2019, 518: 57-65.
[6] WANG F, LI L, ZHU H Z, et al. Effects of heat treatment temperature and CeO₂ content on the phase composition, structure, and properties of monazite phosphate-based glass-ceramics[J]. Journal of Non-Crystalline Solids, 2022, 588: 121631.
[7] KONG L G, KARATCHEVTSEVA I, WEI T. In-situ crystallization of lanthanide titanate stannate (Ln₂TiSnO₇) pyrochlore in glass: a glass-ceramic system for potential nuclear waste sequestration[J]. Journal of Nuclear Materials, 2023, 577: 154322.
[8] CAI X, TENG Y C, WU L, et al. The synthesis and chemical durability of Nd-doped single-phase zirconolite solid solutions[J]. Journal of Nuclear Materials, 2016, 479: 455-460.
[9] KONG L G, KARATCHEVTSEVA I, ZHANG Y J, et al. The incorporation of Nd or Ce in CaZrTi₂O₇ zirconolite: ceramic versus glass-ceramic[J]. Journal of Nuclear Materials, 2021, 543: 152583.
[10] KUMAR YADAV A, GAUTAM C R. A review on crystallisation behaviour of perovskite glass ceramics[J]. Advances in Applied Ceramics, 2014, 113(4): 193-207.
[11] LIVSHITS T S, LIZIN A A, TOMILIN S V. Chemical and radiation stability of ²⁴⁴Cm-doped aluminate perovskite[J]. Geology of Ore Deposits, 2014, 56(6): 440-450.
[12] BARDEZ-GIBOIRE I, KIDARI A, MAGNIN M, et al. Americium and trivalent lanthanides incorporation in high-level waste glass-ceramics[J]. Journal of Nuclear Materials, 2017, 492: 231-238.
[13] LOISEAU P, CAURANT D. Glass-ceramic nuclear waste forms obtained by crystallization of SiO₂-Al₂O₃-CaO-ZrO₂-TiO₂ glasses containing lanthanides (Ce, Nd, Eu, Gd, Yb) and actinides (Th): study of the crystallization from the surface[J]. Journal of Nuclear Materials, 2010, 402(1): 38-54.
[14] KAMEL N E H, MOUHEB Y, KAMEL Z, et al. Influence of the sintering temperature on the Sr content in a Ca_(1-x-y)Ce_xSr_yAl_zTi_(1-z)O₃ perovskite (x=0.04-0.16) Co-doped with Ce[J]. Journal of Nuclear Materials, 2016, 477: 139-148.
[15] MU W J, YU Q H, LI X L, et al. Crystal structure stability of simulated Sr_1-1.5xY_xTiO₃(x=0-0.12) waste forms[J]. Journal of Wuhan University of Technology-Mater Sci Ed, 2017, 32(1): 89-93.
[16] GOETHALS J, BEDIDI A, FOURDRIN C, et al. Experimental study of trivalent rare-earth element incorporation in CaTiO₃ perovskite: evidence for a new substitution mechanism[J]. Physics and Chemistry of Minerals, 2019, 46(10): 1003-1015.
[17] XU Y L, LIAO Q L, WANG F, et al. Impacts of substitution of Fe₂O₃ for SiO₂ on structure and properties of borosilicate glasses containing MoO₃[J]. Journal of Non-Crystalline Solids, 2023, 599: 121982.
[18] ZHOU J J, LIAO Q L, WANG F, et al. Effect of Na₂O and CaO on the solubility and crystallization of Mo in borosilicate glasses[J]. Journal of Non-Crystalline Solids, 2021, 557: 120623.
[19] ZHU H Z, WANG F, LIAO Q L, et al. Effect of CeO₂ and Nd₂O₃ on phases, microstructure and aqueous chemical durability of borosilicate glass-ceramics for nuclear waste immobilization[J]. Materials Chemistry and Physics, 2020, 249: 122936.
[20] AKATOV A A, NIKONOV B S, OMEL'YANENKO B I, et al. Influence of the content of a surrogate of iron aluminate high-level wastes on the phase composition and structure of glassy materials for their immobilization[J]. Glass Physics and Chemistry, 2010, 36(1): 45-52.
[21] ZHU H Z, WANG F, LIAO Q L, et al. Synthesis and characterization of zirconolite-sodium borosilicate glass-ceramics for nuclear waste immobilization[J]. Journal of Nuclear Materials, 2020, 532: 152026.
[22] YU M, LIN J, ZHOU S B, et al. Sol-gel deposition and luminescent properties of oxyapatite Ca₂(Y, Gd)₈(SiO₄)₆O₂ phosphor films doped with rare earth and lead ions[J]. Journal of Materials Chemistry, 2002, 12(1): 86-91.
[23] KSAPABUTR B, GULARI E, WONGKASEMJIT S. Sol-gel derived porous ceria powders using cerium glycolate complex as precursor[J]. Materials Chemistry and Physics, 2006, 99(2/3): 318-324.
[24] LI F, LIU X, HE T. Solid state synthesis of CaTiO₃: Dy³⁺/Eu³⁺ phosphors towards white light emission[J]. Chemical Physics Letters, 2017, 686: 78-82.
[25] YAN Y X, YANG H, YI Z, et al. Design of ternary CaTiO₃/g-C₃N₄/AgBr Z-scheme heterostructured photocatalysts and their application for dye photodegradation[J]. Solid State Sciences, 2020, 100: 106102.
[26] YANG L Q, CAI Z Y, YANG L Q, et al. Solid state synthesis, luminescence and afterglow enhancements of CaTiO₃: Pr³⁺ by Ga³⁺ codoping[J]. Journal of Luminescence, 2018, 197: 339-342.
[27] SADDEEK Y B, GAAFAR M S, BASHIER S A. Structural influence of PbO by means of FTIR and acoustics on calcium alumino-borosilicate glass system[J]. Journal of Non-Crystalline Solids, 2010, 356(20/21/22): 1089-1095.
[28] MARZOUK S Y, SEOUDI R, SAID D A, et al. Linear and non-linear optics and FTIR characteristics of borosilicate glasses doped with gadolinium ions[J]. Optical Materials, 2013, 35(12): 2077-2084.
[29] KOUDELKA L, MOŠNER P, ŠUBÍK J. Study of structure and properties of modified borophosphate glasses[C]//IOP Conference Series: Materials Science and Engineering, 2009, 2: 012015.
[30] TANG Y X, JIANG Z H, SONG X Y. NMR, IR and Raman spectra study of the structure of borate and borosilicate glasses[J]. Journal of Non-Crystalline Solids, 1989, 112(1/2/3): 131-135.
[31] SUTRADHAR M, CARRELLA L M, RENTSCHLER E. Mononuclear Mn(III) and dinuclear Mn(III, III) Schiff base complexes: influence of π-π stacking on magnetic properties[J]. Polyhedron, 2012, 38(1): 297-303.
[32] GU Y X, LIAO Q L, WANG F, et al. Effect of Li₂O substitution for Na₂O on the solubility and water durability of Mo in aluminoborosilicate glass[J]. International Journal of Applied Glass Science, 2022, 13(1): 112-120.
[33] EREMYASHEV V E, OSIPOV A A, OSIPOVA L M. Borosilicate glass structure with rare-earth-metal cations substituted for sodium cations[J]. Glass and Ceramics, 2011, 68(7): 205-208.
[34] GAAFAR M S, MARZOUK S Y. Mechanical and structural studies on sodium borosilicate glasses doped with Er₂O₃ using ultrasonic velocity and FTIR spectroscopy[J]. Physica B: Condensed Matter, 2007, 388(1/2): 294-302.
[35] MALININA G A, STEFANOVSKY S V, STEFANOVSKAYA O I. Phase composition and structure of boron-free and boron-containing sodium aluminum iron silicate glass materials for solid radioactive waste immobilization[J]. Glass Physics and Chemistry, 2012, 38(3): 280-289.
[36] DANTAS N O, AYTA W E F, SILVA A C A, et al. Effect of Fe₂O₃ concentration on the structure of the SiO₂-Na₂O-Al₂O₃-B₂O₃ glass system[J]. Spectrochimica Acta Part A: Molecular and Biomolecular Spectroscopy, 2011, 81(1): 140-143.
[37] WANG Z B, ZHAO Z W, 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.
[38] MD ZAIN S K, SAZALI E S, MOHD-NOOR F, et al. Effect of calcination temperature on structure of mesoporous borosilicate bioglass[J]. Journal of Physics: Conference Series, 2021, 1892(1): 012030.
[39] WANG F, WANG Y L, CHEN J J, et al. Effect of cerium oxide on phase composition, structure, thermal stability and aqueous durability of sodium-iron-boron-phosphate based glasses[J]. Journal of Nuclear Materials, 2021, 556: 153199.
[40] OJOVAN M I, LEE W E. An introduction to nuclear waste immobilisation[M]. 3rd ed. London: Newnes, 2013.
[41] FRANKEL G S, VIENNA J D, LIAN J, et al. Recent advances in corrosion science applicable to disposal of high-level nuclear waste[J]. Chemical Reviews, 2021, 121(20): 12327-12383.
[42] DORET A, PELLERIN N, ALLIX M, et al. Influence of alteration solutions on the chemical durability of the zerodur glass-ceramic: structural investigation[J]. International Journal of Applied Ceramic Technology, 2015, 12(4): 811-822.

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Fe₂O₃对含铈钙钛矿玻璃陶瓷物相结构及化学稳定性的影响

Effect of Fe₂O₃ on Phase Structure and Chemical Stability of Cerium-Containing Perovskite Glass-Ceramics

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