多组元烧绿石陶瓷固化体的制备及其抗浸出性能

滕振; 冯万林; 曾思藩; 陈柏桦; 张海斌; 彭述明

doi:10.7538/hhx.2022.YX.2021098

多组元烧绿石陶瓷固化体的制备及其抗浸出性能

中国工程物理研究院核物理与化学研究所,四川绵阳621999

计量
- 文章访问数: 321
- HTML全文浏览量: 3
- PDF下载量: 2681
出版历程
- 刊出日期: 2022-04-19

Preparation and Leaching Reliability of Multi-Pyrochlore Ceramic Immobilizations Materials

Institute of Nuclear Physics and Chemistry, China Academy of Engineering Physics, Mianyang 621999, China

摘要

摘要: 烧绿石具有优异的理化稳定性和耐辐照稳定性，被认为是理想的放射性核素固化基材。然而，人造烧绿石在烧结过程中对核素的选择性高，从而限制了其固化核素的种类和数量。针对上述问题，本工作以镧系元素铕（Eu）、钐（Sm）、钕（Nd）模拟放射性的锕系核素，成功制备得到了2、3、4组元的烧绿石结构陶瓷固化体。结果表明，目标核素均匀地固溶在烧绿石的晶格结构中形成了单相均一的多组元烧绿石陶瓷固化体。化学浸出实验表明，多组元烧绿石结构具有优异的抗浸出性能，是一种具有应用前景的高放废物陶瓷固化体候选材料。
- 多组元烧绿石 /
- 陶瓷固化体 /
- 高放废物 /
- 抗浸出性能
Abstract: Pyrochlore has been extensively studied as one of the most ideal candidates for nuclear wastes immobilization, due to its excellent geological stability, radiation tolerance, low chemical leaching rate, and high thermal stability. However, the artificial pyrochlore has a relatively high selectivity for curing nuclides, which limits the types and quantity of its target species. To tackle the challenge, a variety of simulated nuclides(Eu, Sm and Nd) were successfully incorporated into the pyrochlore lattice by solid-state reactions. The experimental results show that the multi-pyrochlore exhibits a homogeneous structure with single phase. Leaching tests indicate that the multi-pyrochlore owns excellent leaching resistance and chemical stability, which enables multi-pyrochlore a promising immobilization material for high-level waste.
- multi-pyrochlore /
- ceramic immobilization /
- high-level waste /
- leaching resistance

HTML全文

5669

下载: 全尺寸图片幻灯片

参考文献(36)

[1]	阂茂中.放射性废物处置原理[M].北京:中国原子能出版社，1998.
[2]	Weber W J, Navrotsky A, Stefanovsky S, et al. Materials science of high-level nuclear waste immobilization[J]. MRS Bulletin, 2009, 34(1): 46-53.
[3]	Sengupta P. A review on immobilization of phosphate containing high level nuclear wases within glass matrix-present status and future challenges[J]. J Hazard Mater, 2012, 235: 17-28.
[4]	Stewart D. Geochemical aspects of radioactive waste disposal[M]. Springer Verlag, 1984.
[5]	Chick L, Lokken R, Thomas L. Basalt glass ceramics for the immobilization of transuranic nuclear waste[J]. Bull Am Ceram Soc, 1983, 62(4): 505-516.
[6]	Chun K S, Kim S S, Kang C H. Release of boron and cesium or uranium from simulated borosilicate waste glasses through a compacted Ca-bentonite layer[J]. J Nucl Mater, 2001, 298: 150-154.
[7]	Mccloy J S, Riley B J, Goel A, et al. Rhenium solubility in borosilicate nuclear waste glass: implications for the processing and immobilization of technetium-99[J]. Environ Sci Technol, 2012, 46(22): 12616-12622.
[8]	McKeown D A, Muller I S, Matlack K S, et al. X-ray absorption studies of vanadium valence and local environment in borosilicate waste glasses using vanadium sulfide, silicate, and oxide standards[J]. J Non Cryst Solids, 2002, 298(2-3): 160-175.
[9]	Connelly A J, Travis K P, Hand R J, et al. Composition-structure relationships in simplified nuclear waste glasses: mixed alkali borosilicate glasses[J]. J Am Ceram Soc, 2011, 94(1): 151-159.
[10]	Hatch L P. Ultimate disposal of radioactive wastes[J]. Sci Am, 1953, 41(3): 410-421.
[11]	McMaster S A, Ram R, Faris N, et al. Radionuclide disposal using the pyrochlore supergroup of minerals as a host matrix: a review[J]. J Hazard Mater, 2018, 260: 257-269.
[12]	Foxhall H R, Travis K P, Owens S L. Effect of plutonium doping on radiation damage in zirconolite: a computer simulation study[J]. J Nucl Mater, 2014, 444(1-3): 220-228.
[13]	Kusiak M A, Williams I S, Dunkley D J, et al. Monazite to the rescue: U-Th-Pb dating of the intrusive history of the composite Karkonosze pluton, Bohemian Massif[J]. Chem Geol, 2014, 364(1): 76-92.
[14]	Wang S X, Begg B D, Wang L M, et al. Radiation stability of gadolinium zirconate: a waste form for plutonium disposition[J]. J Mater Res, 1999, 14(12): 4470-4473.
[15]	Lian J, Zu X T, Kutty K V G, et al. Ion-irradiation-induced amorphization of La₂Zr₂O₇ pyrochlore[J]. Phys Rev B, 2002, 66(5): 054108.
[16]	Lang M, Zhang F, Zhang J, et al. Review of A₂B₂O₇ pyrochlore response to irradiation and pressure[J]. Nucl Instrum Methods Phys Res, Sect B, 2010, 268(19): 2951-2959.
[17]	Weber W J, Ewing R C. Plutonium immobilization and radiation effects[J]. Science, 2000, 289(5487): 2051-2062.
[18]	Sickafus K E, Minervini L, Grimes R W, et al. Radiation tolerance of complex oxides[J]. Science, 2000, 289(5480): 748-751.
[19]	Kholghy M, Kharatyan S, Edris H. SHS/PHIP of ceramic composites using ilmenite concentrate[J]. J Alloys Compd, 2010, 502(2): 491-494.
[20]	Wang J, Wang J X, Zhang Y B, et al. Order-disorder phase structure, microstructure and aqueous durability of (Gd, Sm)2(Zr, Ce)2O7 ceramics for immobilizing actinides[J]. Ceram Int, 2019, 45(14): 17898-17904.
[21]	国家环境保护局.GB 7023-86放射性废物固化体长期浸出实验[S].北京：中国标准出版社，1986.
[22]	Lu X R, Fan L, Shu X Y, et al. Phase evolution and chemical durability of co-doped Gd₂Zr₂O₇ ceramics for nuclear waste forms[J]. Ceram Int, 2015, 41(5): 6344-6349.
[23]	Peng L, Zhang K, Yin D, et al. Self-propagating synthesis, mechanical property and aqueous durability of Gd₂Ti₂O₇ pyrochlore[J]. Ceram Int, 2016, 42(16): 18907-18913.
[24]	Lian J, Wang L, Chen J, et al. The order-disorder transition in ion-irradiated pyrochlore[J]. Acta Mater, 2003, 51(5): 1493-1502.
[25]	Teng Z, Zhu L, Tan Y, et al. Synthesis and structures of high-entropy pyrochlore oxides[J]. J Europ Ceram Soc, 2020, 40(4): 1639-1643.
[26]	Vegard L. Die konstitution der mischkristalle und die raumfüllung der atome[J]. Z Med Phys, 1921, 5(1): 17-26.
[27]	Garbout A, Taazayet I B, Férid M. Structural, FT-IR, XRD and Raman scattering of new rare-earth-titanate pyrochlore-type oxides LnEuTi2O7 (Ln=Gd, Dy)[J]. J Alloy Compd, 2013, 573: 43-52.
[28]	Nandi S, Jana Y M, Gupta H C. Lattice dynamical investigation of the Raman and infrared wavenumbers and heat capacity properties of the pyrochlores R₂Zr₂O₇ (R=La, Nd, Sm, Eu)[J]. J Phys Chem Solids, 2018, 115: 347-354.
[29]	Liu K, Zhang K, Deng T, et al. Preparation of Gd₂Zr₂O₇ nanoceramics from two-step thermal treatment and the aqueous durability analysis[J]. Ceram Int, 2020, 46(9): 13040-13046.
[30]	Xu C, Wang L, Bai B, et al. Rapid synthesis of Gd2Zr2O7 ceramics by flash sintering and its aqueous durability[J]. J Eur Ceram Soc, 2020, 40(4): 1620-1625.
[31]	Hu Q, Zeng J, Wang L, et al. Helium ion irradiation effects on neodymium and cerium co-doped Gd₂Zr₂O₇ pyrochlore ceramic[J]. J Rare Earths, 2018, 36(4): 398-403.
[32]	Brown I D. Bond valence theory[J]. Struct Bond, 2014, 158: 11-58.
[33]	Ewing R C, Weber W J, Lian J. Nuclear waste disposal-pyrochlore (A₂B₂O₇): nuclear waste form for the immobilization of plutonium and “minor” actinides[J]. J Appl Phys, 2004, 95(11): 5949-5971.
[34]	Chen S, Liu X, Shu X, et al. Rapid synthesis and chemical durability of Gd₂Zr₂-xCe_xO₇ via SPS for nuclear waste forms[J]. Ceram Int, 2018, 44(16): 20306-20310.
[35]	Zhang K, He Z, Peng L, et al. Self-propagating synthesis of Y_2-xNd_xTi₂O₇ pyrochlore and its aqueous durability as nuclear waste form[J]. Scripta Mater, 2018, 146: 300-303.
[36]	Donald I W, Metcalfe B L, Taylor R. The immobilization of high-level radioactive wastes using ceramics and glasses[J]. J Mater Sci, 1997, 32(22): 5851-5887.