YIG陶瓷对三价锕系模拟核素的固化行为研究

doi:10.15541/jim20210669

无机材料学报 ›› 2022, Vol. 37 ›› Issue (7): 757-763.DOI: 10.15541/jim20210669

所属专题：【结构材料】核用陶瓷

YIG陶瓷对三价锕系模拟核素的固化行为研究

罗世淋¹^,²(), 张胜泰¹, 许保亮¹, 王凌坤¹, 段思逸菡¹, 丁艺¹, 赵倩¹, 段涛¹()

1.西南科技大学核废物与环境安全省部共建协同创新中心, 绵阳 621010
2.西华师范大学物理与空间科学学院, 南充 637002

收稿日期:2021-11-01 修回日期:2022-01-20 出版日期:2022-07-20 网络出版日期:2022-01-24
通讯作者: 段涛, 教授. E-mail: duant@swust.edu.cn
作者简介:罗世淋(1995-), 男, 硕士研究生. E-mail: 13890720525@139.com
基金资助:
国家重点研发计划(2016YFC1402500);国家自然科学基金(41272050);国家自然科学基金(21976148)

Immobilizing Behavior of Trivalent Actinide Nuclides by YIG Ceramics

LUO Shilin¹^,²(), ZHANG Shengtai¹, XU Baoliang¹, WANG Lingkun¹, DUAN Siyihan¹, DING Yi¹, ZHAO Qian¹, DUAN Tao¹()

1. National Co-Innovation Center for Nuclear Waste Disposal and Environmental Safety, Southwest University of Science and Technology, Mianyang 621010, China
2. Physics and Space Sciences College, China West Normal University, Nanchong 637002, China

Received:2021-11-01 Revised:2022-01-20 Published:2022-07-20 Online:2022-01-24
Contact: DUAN Tao, professor. E-mail: duant@swust.edu.cn
About author:LUO Shilin (1995-), male, Master candidate. E-mail: 13890720525@139.com
Supported by:
National Key R&D Program of China(2016YFC1402500);National Natural Science Foundation of China(41272050);National Natural Science Foundation of China(21976148)

摘要/Abstract

摘要：

石榴石具有较大的锕系包容量及化学灵活性, 被认为是潜在的锕系核素固化基材。本工作以Nd³⁺模拟三价锕系核素, 通过高温固相法成功合成了Y_3-_xNd_xFe₅O₁₂(0≤x≤2)系列钇铁石榴石(YIG)固化体。研究了Nd在YIG固化体中的固溶极限和Nd掺杂量对固化体的物相和微观结构的影响规律, 以及不同pH条件下Nd掺杂钇铁石榴石固化体的化学耐久性。研究结果表明, 当x≤1.7时, YIG基固化体为纯相YIG; 当x≥1.8时, YIG基固化体中YIG、NdFeO₃和Fe₂O₃三相共存。纯相YIG基固化体对Nd³⁺的固溶极限约为29.5%(质量分数)。随着Nd掺杂量增加, 固化体的密度增大, 体积减小, 孔隙率减小。浸出实验结果显示, 28 d后元素归一化浸出率(LR_i)逐渐趋于平衡, 42 d后, 其元素的LR_i为10^-6~10^-5g·m^-2·d^-1。LR_Y小于LR_Nd, 且酸性溶液中元素归一化浸出率也略高于中性和碱性溶液。这些结果表明, YIG陶瓷是理想的三价锕系核素候选固化基材。

关键词: 钇铁石榴石(YIG), 锕系核素, 相演变, 化学稳定性

Abstract:

Garnet is considered as a potential matrix for immobilizing high-level radioactive waste (HLW) because of its large actinide package capacity and chemical flexibility. Y_3-_xNd_xFe₅O₁₂ (0≤x≤2) series yttrium iron garnet (YIG) samples was successfully synthesized by solid-state sintering method using Nd³⁺ to simulate trivalent actinides. The solubility limit of Nd in the YIG and the influence of Nd doping amount on the phase and microstructure of ceramics was studied. Then the chemical durability of Nd-doped yttrium iron garnet solidified body under different pH conditions was evaluated. The results show that the ceramics with x≤1.7 show homogeneous single YIG, but the ceramics with x≥1.8 exhibit coexistence of three crystal phases (YIG, NdFeO₃ and Fe₂O₃). The solubility limit of Nd³⁺ in the pure YIG is about 29.5% (in mass). As the amount of Nd doping increases, the density of the ceramics increases, the volume decreases, and the porosity decreases. The leaching experiment results show that the normalized leaching rate of the elements (LR_i) is 10^-6~10^-5g·m^-2·d^-1. LR_Y is smaller than LR_Nd, and the normalized leaching rate of the elements in acid leachate is slightly higher than those in neutral and alkaline leachates. The results indicate that YIG ceramics are a potential candidate form for trivalent actinides.

Key words: yttrium iron garnet (YIG), actinide, phase evolution, chemical stability

中图分类号:

TQ174

罗世淋, 张胜泰, 许保亮, 王凌坤, 段思逸菡, 丁艺, 赵倩, 段涛. YIG陶瓷对三价锕系模拟核素的固化行为研究[J]. 无机材料学报, 2022, 37(7): 757-763.

LUO Shilin, ZHANG Shengtai, XU Baoliang, WANG Lingkun, DUAN Siyihan, DING Yi, ZHAO Qian, DUAN Tao. Immobilizing Behavior of Trivalent Actinide Nuclides by YIG Ceramics[J]. Journal of Inorganic Materials, 2022, 37(7): 757-763.

图/表 8

图1 (a) Y3-xNdxFe5O12(0≤x≤2.0)(大浓度梯度)和(b) Y3-xNdxFe5O12(1.7≤x≤2.0)(小浓度梯度)样品的XRD图谱

Fig. 1 XRD pattern of (a) Y3-xNdxFe5O12 (0≤x≤2.0, large gradient) and (b) Y3-xNdxFe5O12 (1.7≤x≤2.0, small gradient)

图2 Y3-xNdxFe5O12(0≤x<2)晶胞参数随Nd固溶量的变化趋势

Fig. 2 Variation trend of lattice parameter of Y3-xNdxFe5O12 (0≤x<2) with Nd amount

图3 Y3-xNdxFe5O12(0≤x≤2)样品的SEM照片(a) x=0, (b) x=0.5, (c) x=1.5, (d) x=2.0及其(e, f)EDS点分析

Fig. 3 SEM images of Y3-xNdxFe5O12 (0≤x≤2) when (a) x=0, (b) x=0.5, (c) x=1.5, (d) x=2.0, and (e, f) EDS analyses of corresponding spots in (d)

图4 x=1.5样品的EDS元素分布图谱

Fig. 4 EDS elements mappings of the sample x=1.5 Colorful figures are available on website

图5 Y3-xNdxFe5O12(0≤x≤2)样品的(a)密度和线性伸缩率, (b)相对密度和孔隙率

Fig. 5 (a) Density and linear shrinkage, (b) relative density and open porosity of Y3-xNdxFe5O12 (0≤x≤2)

图6 Y1.5Nd1.5Fe5O12陶瓷在不同pH浸出剂中(a)Y和(b)Nd的归一化浸出率

Fig. 6 Normalized release rates of (a) Y and (b) Nd in Y1.5Nd1.5Fe5O12 ceramics in the leaching solution with different pH

表1 几种不同石榴石浸出率对比

Table 1 Normalized release rates of several different garnets

Material	Normalized release rate/(g·m^-2·d^-1)	Ref.
Ca_1.59Gd_1.01Ce_0.45Zr_1.14Fe_0.77Fe_3.03O₁₂	10^-6-10^-3	[7]
LuAG, YAG	10^-5-10^-4	[28]
(Ca_1.5GdTh_0.5)(ZrFe)(Fe₃)O₁₂	10^-6-10^-3	[29]
Ce-doped YIG	10^-5-10^-4	[30]
YIG	10^-6-10^-5	In this work

图7 Y1.5Nd1.5Fe5O12陶瓷浸出后的SEM照片

Fig. 7 SEM images of Y1.5Nd1.5Fe5O12 ceramics after leaching (a) pH 3; (b) pH 7; (c) pH 11

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YIG陶瓷对三价锕系模拟核素的固化行为研究

Immobilizing Behavior of Trivalent Actinide Nuclides by YIG Ceramics

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