Citation: XIA Xiang-Lai, LI Lin-Yan, GUO Fang, SU Wei, LIU Yan, CHEN Xiao-Mou, PAN She-Qi. Simulation of the Immobilization of Pu in the Gd₂Zr₂O₇ Matrix by Investigating the Thermophysical Properties of (Gd_1-xCe_x)₂Zr₂O_7+x[J]. Acta Physico-Chimica Sinica, ;2015, 31(9): 1810-1814. doi: 10.3866/PKU.WHXB201507203 shu

Simulation of the Immobilization of Pu in the Gd₂Zr₂O₇ Matrix by Investigating the Thermophysical Properties of (Gd_1-xCe_x)₂Zr₂O_7+x

XIA Xiang-Lai ^1,2 ,
LI Lin-Yan ^2, ,
GUO Fang ^1, ,
SU Wei ³ ,
LIU Yan ³ ,
CHEN Xiao-Mou ³ ,
PAN She-Qi ³

1.
1 College of Chemistry, Liaoning University, Shenyang 110036, P. R. China;
2 Institute of Nuclear and New Energy Technology, Tsinghua University, Beijing 100084, P. R. China;
3 China Academy of Engineering Physics, Mianyang 621900, Sichuan Province, P. R. China

Received Date: 26 March 2015
Available Online: 20 July 2015
Fund Project: 国家自然科学基金委员会和中国工程物理研究院联合基金(11176014) (11176014)国家自然科学基金(21471088)资助项目 (21471088)

Polycrystalline samples of (Gd_1-xCe_x)₂Zr₂O_7+x (0 ≤ x ≤ 0.7) were synthesized by solid-state reaction using NaF as a flux at 1000 ℃ to simulate Pu-immobilization in the Gd₂Zr₂O₇ matrix. Phase transformation and variation of the thermal expansion coefficients (TECs) and thermal conductivities (TCs) of the samples with temperature and composition were investigated. Powder X-ray diffraction (XRD) patterns show that pure Gd₂Zr₂O₇ has a weakly ordered pyrochlore structure, whereas Ce-containing samples (i.e., the Pu-simulated solidified samples) exhibit a defect fluorite structure even if x is as low as 0.1. When x reaches 0.7, the XRD peaks of these samples widen. In the Ce 3d X-ray photoelectron spectrum (XPS) of (Gd_1-xCe_x)₂Zr₂O_7+x there are six peaks located at binding energies of 881.7, 888.1, 897.8, 900.4, 907.1, and 916.1 eV, which are almost the same as the peaks of CeO2. The Ce 3d XPS reveals that the Ce species in (Gd_1-xCe_x)₂Zr₂O_7+x are tetravalent. The TECs of (Gd_1-xCe_x)₂Zr₂O_7+x (0 ≤ x ≤ 0.7) generally increase with increasing temperature. At the same temperature, the TECs and TCs exhibit the same variation trend with the composition of the simulated solidified forms: they decrease from x = 0 to 0.1 and then linearly increase from x = 0.1 to 0.7.
- Immobilization of nuclear waste,
- Pyrochlore structure,
- Defect fluorite structure,
- Thermal expansion coefficient,
- Thermal conductivity
1. [1]
  
  (1) Stefanovsky, S. V.; Yudintsev, S. V.; Livshits, T. S. IOP Conf. Series: Mater. Sci. Eng. 2010, 9, 012001-1. doi: 10.1088/1757-899X/9/1/012001
2. [2]
  (2) Yudintsev, S. V.; Stefanovsky, S. V.; Ewing, R. C. Actinide Host Phases as Radioactive Waste Forms. In Structural Chemistry of Inorganic Actinide Compounds; Krivovichev, S. V., Burns, P. C., Tananaev, I. G. Eds.; Elsevier: Amsterdam, 2007; pp 457-490.
3. [3]
  (3) Donald, I. W.; Metcalfe, B. L.; Taylor, R. N. J. J. Mater. Sci. 1997, 32, 5851. doi: 10.1023/A:1018646507438
4. [4]
  (4) Lutze, W.; Ewing, R. C. Radioactive Waste Forms for the Future; Lutze, W., Ewing, R. C. Eds.; Elsevier: Amsterdam, 1988; pp 1-159.
5. [5]
  (5) Kumar, B.; Lin, S. J. Am. Ceram. Soc. 1991, 74, 226. doi: 10.1111/jace.1991.74.issue-1
6. [6]
  (6) Stefanovsky, S. V.; Ivanov, I. A.; Gulin, A. N. Scientific Basis for Nuclear Waste Management XVIII; Murakami, T., Ewing, R. C. Eds.; Materials Research Society: Pittsburgh, PA, 1995; pp 101-106.
7. [7]
  (7) Sickafus, K. E.; Minervini, L.; Grimes, R. W.; Valdez, J. A.; Ishimaru, M.; Li, F.; McClellan, K. J.; Hartmann, T. Science 2000, 289, 748. doi: 10.1126/science.289.5480.748
8. [8]
  (8) Weber, W. J.; Ewing, R. C. Science 2000, 289, 2051. doi: 10.1126/science.289.5487.2051
9. [9]
  (9) Lu, X. R.; Dong, F. Q.; Hu, S.; Wang, X. L.; Wu, Y. L. Acta Phys. Sin. 2012, 61, 152401-1. [卢喜瑞, 董发勤, 胡淞, 王晓丽, 吴彦霖. 物理学报, 2012, 61, 152401-1.]
10. [10]
  (10) Zhang, F. X.; Wang, J. W.; Lian, J.; Lang, M. K.; Becker, U.; Ewing, R. C. Phys. Rev. Lett. 2008, 100, 045503-1. doi: 10.1103/PhysRevLett.100.045503
11. [11]
  (11) Mandal, B. P.; Pandey, M.; Tyagi, A. K. J. Nucl. Mater. 2010, 406, 238. doi: 10.1016/j.jnucmat.2010.08.042
12. [12]
  (12) Kutty, K. V. G.; Asuvathraman, R.; Madhavan, R. R.; Jena, H. J. Phys. Chem. Solids 2005, 66, 596. doi: 10.1016/j.jpcs.2004.06.066
13. [13]
  (13) Weber, W. J.; Wald, J. W.; Matzke, H. J. Nucl. Mater. 1986, 138, 196. doi: 10.1016/0022-3115(86)90006-1
14. [14]
  (14) Kerdaniel, E. D. F.; Clavier, N.; Dacheux, N.; Terra, O.; Podor, R. J. Nucl. Mater. 2007, 362, 451. doi: 10.1016/j.jnucmat.2007.01.132
15. [15]
  (15) Metcalfe, B. L.; Donald, I. W.; Fong, S. K.; Gerrard, L. A.; Strachan, D. M.; Scheele, R. D. J. Nucl. Mater. 2009, 385, 485. doi: 10.1016/j.jnucmat.2008.12.035
16. [16]
  (16) Ringwood, A. E.; Kesson, S. E.; Ware, N. G.; Hibberson, W.; Major, A. Nature 1979, 278, 219. doi: 10.1038/278219a0
17. [17]
  (17) Patwe, S. J.; Ambekar, B. R.; Tyagi, A. K. J. Alloy. Compd. 2005, 389, 243. doi: 10.1016/j.jallcom.2004.06.094
18. [18]
  (18) Tang, J. Y.; Chen, X. M.; Pan, S. Q.; Mu, T.; He, D. W. At. Energy Sci. Technol. 2010, 44, 394. [唐敬友, 陈晓谋, 潘社奇, 牟涛, 贺端威. 原子能科学技术, 2010, 44, 394.]
19. [19]
  (19) Lu, X. R.; Ding, Y.; Dan, H.; Yuan, S. B.; Mao, X. L.; Fan, L.; Wu, Y. L. Ceram. Int. 2014, 40, 13191. doi: 10.1016/j.ceramint.2014.05.024
20. [20]
  (20) Mandal, B. P.; Garg, N.; Sharma, S. M.; Tyagi, A. K. J. Nucl. Mater. 2009, 392, 95. doi: 10.1016/j.jnucmat.2009.03.050
21. [21]
  (21) Reid, D. P.; Stennettn, M. C.; Hyatt, N. C. J. Solid State Chem. 2012, 191, 2. doi: 10.1016/j.jssc.2011.12.039
22. [22]
  (22) Dickson, C. L.; Glasser, F. P. Cem. Concr. Res. 2000, 30, 1619. doi: 10.1016/S0008-8846(00)00362-8
23. [23]
  (23) Lu, X. R.; Fan, L.; Shu, X. Y.; Su, S. J.; Ding, Y.; Yi, F. C. Ceram. Int. 2015, 41, 6344. doi: 10.1016/j.ceramint.2015.01.068
24. [24]
  (24) Zhao, P. Z.; Li, L.Y.; Xu, S. M.; Zhang, Q. Acta Phys. -Chim. Sin. 2013, 29, 1168. [赵培柱, 李林艳, 徐盛明, 张覃. 物理化学学报, 2013, 29, 1168.] doi: 10.3866/PKU.WHXB201304013
25. [25]
  (25) Zhao, L. Z. Acta Phys. Sin. 1989, 38, 987. [赵良仲. 物理学报, 989, 38, 987.]
26. [26]
  (26) Zhang, H. S.; Chen, X. G.; Li, G.; Wang, X. L.; Dang, X. D. J. Eur. Ceram. Soc. 2012, 32, 3693. doi: 10.1016/j.jeurceramsoc.2012.06.003
1. [1]
  Yan Liu , Yuexiang Zhu , Luhua Lai . Introduction to Blended and Small-Class Teaching in Structural Chemistry: Exploring the Structure and Properties of Crystals. University Chemistry, 2024, 39(3): 1-4. doi: 10.3866/PKU.DXHX202306084
2. [2]
  Zitong Chen , Zipei Su , Jiangfeng Qian . Aromatic Alkali Metal Reagents: Structures, Properties and Applications. University Chemistry, 2024, 39(8): 149-162. doi: 10.3866/PKU.DXHX202311054
3. [3]
  Kun WANG , Wenrui LIU , Peng JIANG , Yuhang SONG , Lihua CHEN , Zhao DENG . Hierarchical hollow structured BiOBr-Pt catalysts for photocatalytic CO₂ reduction. Chinese Journal of Inorganic Chemistry, 2024, 40(7): 1270-1278. doi: 10.11862/CJIC.20240037
4. [4]
  Haitang WANG , Yanni LING , Xiaqing MA , Yuxin CHEN , Rui ZHANG , Keyi WANG , Ying ZHANG , Wenmin WANG . Construction, crystal structures, and biological activities of two Ln^Ⅲ₃ complexes. Chinese Journal of Inorganic Chemistry, 2024, 40(8): 1474-1482. doi: 10.11862/CJIC.20240188
5. [5]
  Dongju Zhang . Exploring the Descriptions and Connotations of Basic Concepts of Teaching Crystal Structures. University Chemistry, 2024, 39(3): 18-22. doi: 10.3866/PKU.DXHX202304003
6. [6]
  Weina Wang , Fengyi Liu , Wenliang Wang . “Extracting Commonality, Delving into Typicals, Deriving Individuality”: Constructing a Knowledge Graph of Crystal Structures. University Chemistry, 2024, 39(3): 36-42. doi: 10.3866/PKU.DXHX202308029
7. [7]
  Ji Qi , Jianan Zhu , Yanxu Zhang , Jiahao Yang , Chunting Zhang . Visible Color Change of Copper (II) Complexes in Reversible SCSC Transformation: The Effect of Structure on Color. University Chemistry, 2024, 39(3): 43-57. doi: 10.3866/PKU.DXHX202307050
8. [8]
  Wenyan Dan , Weijie Li , Xiaogang Wang . The Technical Analysis of Visual Software ShelXle for Refinement of Small Molecular Crystal Structure. University Chemistry, 2024, 39(3): 63-69. doi: 10.3866/PKU.DXHX202302060
9. [9]
  Junqiao Zhuo , Xinchen Huang , Qi Wang . Symbol Representation of the Packing-Filling Model of the Crystal Structure and Its Application. University Chemistry, 2024, 39(3): 70-77. doi: 10.3866/PKU.DXHX202311100
10. [10]
  Hongwei Ma , Hui Li . Three Methods for Structure Determination from Powder Diffraction Data. University Chemistry, 2024, 39(3): 94-102. doi: 10.3866/PKU.DXHX202310035
11. [11]
  Yanxin Wang , Hongjuan Wang , Yuren Shi , Yunxia Yang . Application of Python for Visualizing in Structural Chemistry Teaching. University Chemistry, 2024, 39(3): 108-117. doi: 10.3866/PKU.DXHX202306005
12. [12]
  Guoxian Zhu , Jing Chen , Rongkai Pan . Enhancing the Teaching Quality of Atomic Structure: Insights and Strategies. University Chemistry, 2024, 39(3): 376-383. doi: 10.3866/PKU.DXHX202305027
13. [13]
  Xuyang Wang , Jiapei Zhang , Lirui Zhao , Xiaowen Xu , Guizheng Zou , Bin Zhang . Theoretical Study on the Structure and Stability of Copper-Ammonia Coordination Ions. University Chemistry, 2024, 39(3): 384-389. doi: 10.3866/PKU.DXHX202309065
14. [14]
  Tianyun Chen , Ruilin Xiao , Xinsheng Gu , Yunyi Shao , Qiujun Lu . Synthesis, Crystal Structure, and Mechanoluminescence Properties of Lanthanide-Based Organometallic Complexes. University Chemistry, 2024, 39(5): 363-370. doi: 10.3866/PKU.DXHX202312017
15. [15]
  Zhiguang Xu , Xuan Xu , Qiong Luo , Ganquan Wang , Bin Peng . Reform and Practice of Online and Offline Blended Teaching in Structural Chemistry Course. University Chemistry, 2024, 39(6): 195-200. doi: 10.3866/PKU.DXHX202310112
16. [16]
  Jin Jia , Shangda Jiang . Is the z Axis Special in Atomic Structure?. University Chemistry, 2024, 39(6): 400-404. doi: 10.12461/PKU.DXHX202403091
17. [17]
  Wen Shi , Zhangwen Wei , Mei Pan , Chengyong Su . Explorations on the Course Construction of Structural Chemistry Practice and Application Targeting the Chemistry “101 Plan”. University Chemistry, 2024, 39(10): 96-100. doi: 10.12461/PKU.DXHX202409036
18. [18]
  Jingjing QING , Fan HE , Zhihui LIU , Shuaipeng HOU , Ya LIU , Yifan JIANG , Mengting TAN , Lifang HE , Fuxing ZHANG , Xiaoming ZHU . Synthesis, structure, and anticancer activity of two complexes of dimethylglyoxime organotin. Chinese Journal of Inorganic Chemistry, 2024, 40(7): 1301-1308. doi: 10.11862/CJIC.20240003
19. [19]
  Peng ZHOU , Xiao CAI , Qingxiang MA , Xu LIU . Effects of Cu doping on the structure and optical properties of Au₁₁(dppf)₄Cl₂ nanocluster. Chinese Journal of Inorganic Chemistry, 2024, 40(7): 1254-1260. doi: 10.11862/CJIC.20240047
20. [20]
  Asif Hassan Raza , Shumail Farhan , Zhixian Yu , Yan Wu . 用于高效制氢的双S型ZnS/ZnO/CdS异质结构光催化剂. Acta Physico-Chimica Sinica, 2024, 40(11): 2406020-. doi: 10.3866/PKU.WHXB202406020

Get Citation

PDF

XML

Metrics

PDF Downloads(216)
Abstract views(731)
HTML views(43)

通讯作者: 陈斌, bchen63@163.com

1.
沈阳化工大学材料科学与工程学院沈阳 110142

Simulation of the Immobilization of Pu in the Gd2Zr2O7 Matrix by Investigating the Thermophysical Properties of (Gd1-xCex)2Zr2O7+x

Metrics

通讯作者: 陈斌, bchen63@163.com

Simulation of the Immobilization of Pu in the Gd₂Zr₂O₇ Matrix by Investigating the Thermophysical Properties of (Gd_1-xCe_x)₂Zr₂O_7+x