Uranium chemical species in LiCl-KCl eutectic under different conditions for the dissolution of U3O8

被引:16
作者
Liu, Yi-Chuan [1 ,2 ]
Liu, Ya-Lan [1 ]
Wang, Lin [1 ]
Zhong, Yu-Ke [1 ]
Li, Mei [2 ]
Han, Wei [2 ]
Zhao, Yuan [3 ]
Zhou, Tong [3 ]
Zou, Qing [3 ]
Zeng, Xian [3 ]
Shi, Wei-Qun [1 ]
机构
[1] Chinese Acad Sci, Inst High Energy Phys, Lab Nucl Energy Chem, Beijing 100049, Peoples R China
[2] Harbin Engn Univ, Coll Mat Sci & Chem Engn, Key Lab Superlight Mat & Surface Technol, Minist Educ, Harbin 150001, Peoples R China
[3] China Gen Nucl Power Corp, China Nucl Power Technol Res Inst Co Ltd, Reactor Engn & Safety Res Ctr, Shenzhen 518000, Peoples R China
基金
国家自然科学基金重大项目;
关键词
Chemical species; U3O8; NH4Cl; LiCl-KCl; Dissolution; WATER REACTOR-FUEL; RARE-EARTH-OXIDES; ELECTROLYTIC REDUCTION; X-RAY; OXIDATION-STATES; UO2; CHLORIDE; CHLORINATION; SEPARATION; ACTINIDES;
D O I
10.1016/j.jnucmat.2020.152475
中图分类号
T [工业技术];
学科分类号
08 ;
摘要
As a typical uranium oxide, the electrochemical behaviors of U3O8 in molten salt have attracted many research endeavors, but its dissolution behavior and related mechanism in molten salt has been less well understood. In this work, we reported the dissolution of U3O8 in LiCl-KCl eutectic with the assistance of NH4Cl, which has potential significance for the pyrochemical reprocessing of spent oxide fuels. The spectroscopic techniques such as fluorescence emission spectroscopy, UV-Vis absorption spectroscopy, and X-ray Absorption Fine Structure (XAFS) were used to determine the chemical species during the dissolution process of U3O8. The results show that U3O8 can be completely dissolved in molten salt under the air atmosphere, and it exists in the form of [UO2Cl4](2-). In contrast, under an argon atmosphere, the soluble [UO2Cl4](3-) and insoluble UO2 were detected as the main products. (C) 2020 Elsevier B.V. All rights reserved.
引用
收藏
页数:9
相关论文
共 44 条
[1]   Use of HERFD-XANES at the U L3- and M4-Edges To Determine the Uranium Valence State on [Ni(H2O)4]3[U(OH,H2O)(UO2)8O12(OH)3] [J].
Bes, Rene ;
Rivenet, Murielle ;
Solari, Pier-Lorenzo ;
Kvashnina, Kristina O. ;
Scheinost, Andreas C. ;
Martin, Philippe M. .
INORGANIC CHEMISTRY, 2016, 55 (09) :4260-4270
[2]   Uranium oligomerization in chloride-based high temperature melts:: In situ XAS studies [J].
Bhatt, AI ;
de Kerdaniel, ED ;
Kinoshita, H ;
Livens, FR ;
May, I ;
Polovov, IB ;
Sharrad, CA ;
Volkovich, VA ;
Charnock, JM ;
Lewin, RG .
INORGANIC CHEMISTRY, 2005, 44 (01) :2-4
[3]   Solubilities of uranium(IV) dioxide in magnesium chloride, calcium chloride, and aluminum chloride melts: A comparative study [J].
Dai, S ;
Toth, LM ;
DelCul, GD ;
Metcalf, DH .
JOURNAL OF PHYSICAL CHEMISTRY, 1996, 100 (01) :220-223
[4]  
Fujii T., 2016, PROJECT 5 STUDIES AC
[5]   OXIDATION STATES AND COMPLEX IONS OF URANIUM IN FUSED CHLORIDES AND NITRATES [J].
GRUEN, DM ;
MCBETH, RL .
JOURNAL OF INORGANIC & NUCLEAR CHEMISTRY, 1959, 9 (3-4) :290-301
[6]   Electrolytic reduction of spent nuclear oxide fuel as part of an integral process to separate and recover actinides from fission products [J].
Herrmann, S. D. ;
Li, S. X. ;
Simpson, M. F. ;
Phongikaroon, S. .
SEPARATION SCIENCE AND TECHNOLOGY, 2006, 41 (10) :1965-1983
[7]   SEPARATION AND RECOVERY OF URANIUM METAL FROM SPENT LIGHT WATER REACTOR FUEL VIA ELECTROLYTIC REDUCTION AND ELECTROREFINING [J].
Herrmann, S. D. ;
Li, S. X. .
NUCLEAR TECHNOLOGY, 2010, 171 (03) :247-265
[8]   Electrolytic reduction of spent light water reactor fuel - Bench-scale experiment results [J].
Herrmann, Steven ;
Li, Shelly ;
Simpson, Michael .
JOURNAL OF NUCLEAR SCIENCE AND TECHNOLOGY, 2007, 44 (03) :361-367
[9]   Separation and Recovery of Uranium and Group Actinide Products From Irradiated Fast Reactor MOX Fuel via Electrolytic Reduction and Electrorefining [J].
Herrmann, Steven D. ;
Li, Shelly X. ;
Westphal, Brian R. .
SEPARATION SCIENCE AND TECHNOLOGY, 2012, 47 (14-15) :2044-2059
[10]   Chlorination of uranium oxides with CCl4 using a mechanochemical method [J].
Kitawaki, Shinichi ;
Nagai, Takayuki ;
Sato, Nobuaki .
JOURNAL OF NUCLEAR MATERIALS, 2013, 439 (1-3) :212-216