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1.中国科学院上海应用物理研究所 嘉定园区 上海 201800
2.中国科学院大学 北京 100049
Received:17 March 2018,
Revised:23 April 2018,
Published:10 July 2018
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Chunyu XIE, Hanjie CAO, Zenghui YUE, et al. Study on the microstructure of Th1-
Chunyu XIE, Hanjie CAO, Zenghui YUE, et al. Study on the microstructure of Th1-
钍铀混合氧化物存在于钍基核燃料循环的各个阶段,其熔点、溶解性、氧化还原等物理化学性能与微观结构之间存在密切联系。为了宏观模拟钍铀混合氧化物的物理化学性能和提供相关的微观结构实验数据,我们利用同步辐射X射线吸收精细结构(X-ray Absorption Fine Structure,XAFS)谱技术,获取了共沉淀法制备的Th
1-
x
U
x
O
2+
y
混合氧化物样品的钍和铀的局域结构。Th和U的L
3
边XAFS实验数据表明:Th
1-
x
U
x
O
2+
y
的主导结构是ThO
2
成分与局域U
3
O
8
成分的微观混合。对Th
0.8
U
0.2
O
2+
y
样品的扩展X射线吸收谱(Extended X-ray Adsorption Fine Structure,EXAFS)实验数据进行深入分析表明:Th-U相互作用的存在使得ThO
2
成分的Th-Th/U键长与纯ThO
2
相比缩短0.003 nm,同时,局域U
3
O
8
成分的平均U-O键长与纯U
3
O
8
相比增加约0.01 nm。
Background
2
Thorium-uranium mixed oxides exist in different stages of the thorium fuel cycle. The physicochemical properties of Th-U mixed oxides
such as melting point
solubility
and oxido-reduction
are closely related to their microstructures.
Purpose
2
This study aims to study the microstructure of the Th-U mixed oxides by X-ray absorption fine structure (XAFS) technique. In order to macroscopically simulate the physical and chemical properties of Th-U mixed oxides
relevant microstructure data are provided.
Methods
2
The local structures of Th and U in as-prepared Th
1-
x
U
x
O
2+
y
samples are obtained by XAFS spectroscopy technique.
Results
2
The Th and U L
3
-edge XAFS data shows that the dominant structure in Th
1-
x
U
x
O
2+
y
is the mixture of ThO
2
component and local U
3
O
8
component. The extended X-ray adsorption fine structure (EXAFS) data of Th
0.8
U
0.2
O
2+
y
sample is further analyzed. The result shows that there is Th-U interaction in Th
0.8
U
0.2
O
2+
y
sample. The Th-U interaction results that the Th-Th/U bond length in Th
0.8
U
0.2
O
2+
y
slight shorter than that of pure ThO
2
and the U-O bond length in Th
0.8
U
0.2
O
2+
y
larger than that of pure U
3
O
8
.
Conclusion
2
The XAFS technique can supply complementary structure information of Th-U mixed oxides
such as the local structure of Th and U.
E Myllykyla , L Koivula , M Tanhua-Tyrkko , . Direct alpha spectrometry for analysing leached ThO 2 pellets . Journal of Nuclear Materials , 2017 . 493 69 - 76 . DOI: 10.1016/j.jnucmat.2017.06.003 http://doi.org/10.1016/j.jnucmat.2017.06.003 http://cn.bing.com/academic/profile?id=62c3cc7256fc5800c91398ac0043e452&encoded=0&v=paper_preview&mkt=zh-cn .
R Vauchy , R C Belin , A C Robisson , . Actinide oxidation state and OM ratio in hypostoichiometric uranium-plutonium-americium U0.750Pu0.246Am0.004 O 2- x mixed oxides . Inorganic Chemistry , 2016 . 55 ( 5 ): 2123 - 2132 . DOI: 10.1021/acs.inorgchem.5b02533 http://doi.org/10.1021/acs.inorgchem.5b02533 http://europepmc.org/abstract/MED/26907589 .
J J Ma , J G Du , M J Wan , . Molecular dynamics study on thermal properties of ThO 2 doped with U and Pu in high temperature range . Journal of Alloys and Compounds , 2015 . 627 476 - 482 . DOI: 10.1016/j.jallcom.2014.11.223 http://doi.org/10.1016/j.jallcom.2014.11.223 https://www.researchgate.net/publication/272391127_Molecular_dynamics_study_on_thermal_properties_of_ThO2_doped_with_U_and_Pu_in_high_temperature_range .
M Strach , R C Belin , J C Richaud , . Influence of phase separation on the oxidation of (U, Pu)O 2- x . Journal of Physical Chemistry C , 2015 . 119 ( 40 ): 23159 - 23167 . DOI: 10.1021/acs.jpcc.5b07407 http://doi.org/10.1021/acs.jpcc.5b07407 https://www.researchgate.net/publication/283198290_Influence_of_Phase_Separation_on_the_Oxidation_of_UPuO_2-_x .
P Ghosh , N Kuganathan , C Galvin , . Melting behavior of (Th, U)O 2 and (Th, Pu)O 2 mixed oxides . Journal of Nuclear Materials , 2016 . 479 112 - 122 . DOI: 10.1016/j.jnucmat.2016.06.037 http://doi.org/10.1016/j.jnucmat.2016.06.037 http://cn.bing.com/academic/profile?id=2e853fc54ee48a145462d9b7c5aff8ed&encoded=0&v=paper_preview&mkt=zh-cn .
X D Wen , R L Martin , L E Roy , . Effect of spin-orbit coupling on the actinide dioxides AnO 2 (An=Th, Pa, U, Np, Pu, and Am):a screened hybrid density functional study . Journal of Chemical Physics , 2012 . 137 ( 15 ): 416 DOI: 10.1063/1.4757615 http://doi.org/10.1063/1.4757615 http://www.ncbi.nlm.nih.gov/pubmed/23083184 .
L Petit , A Svane , Z Szotek , . Electronic structure and ionicity of actinide oxides from first principles . Physical Review B , 2010 . 81 ( 4 ): 045108 DOI: 10.1103/PhysRevB.81.045108 http://doi.org/10.1103/PhysRevB.81.045108 http://cn.bing.com/academic/profile?id=cb24a93d8f434a0a656db6b58d401d14&encoded=0&v=paper_preview&mkt=zh-cn .
I R Shein , A L Ivanovskii . Thorium compounds with non-metals:electronic structure, chemical bond, and physicochemical properties . Journal of Structural Chemistry , 2018 . 49 ( 2 ): 348 - 370 . DOI: 10.1007/s10947-008-0134-0 http://doi.org/10.1007/s10947-008-0134-0 https://link.springer.com/article/10.1007/s10947-008-0134-0 .
V Neck , M Altmaier , R Muller , . Solubility of crystalline thorium dioxide . Radiochimica Acta , 2003 . 91 ( 5 ): 253 - 262 . DOI: 10.1524/ract.91.5.253.20306 http://doi.org/10.1524/ract.91.5.253.20306 http://cn.bing.com/academic/profile?id=9b28a524bbd3e83d77f8ac612665ea1a&encoded=0&v=paper_preview&mkt=zh-cn .
J Purans , G Heisbourg , N Dacheux , . XAFS study of local structure with picometer accuracy:Th 1- x U x O 2 and Th 1- x Pu x O 2 solid solutions . Physica Scripta , 2015 . T115 925 - 927 . DOI: 10.1238/Physica.Topical.115a00925 http://doi.org/10.1238/Physica.Topical.115a00925 http://www.researchgate.net/publication/278288492_XAFS_study_of_local_structure_with_picometer_accuracy_Th(1-x)UxO(2)_and_Th1-x_PuxO(2)_solid_solutions .
P Cakir , R Eloirdi , F Hubei , . Thorium effect on the oxidation of uranium:photoelectron spectroscopy (XPS/UPS) and cyclic voltammetry (CV) investigation on (U 1- x Th x )O 2 ( x =0 to 1) thin films . Applied Surface Science , 2017 . 393 204 - 211 . DOI: 10.1016/j.apsusc.2016.10.010 http://doi.org/10.1016/j.apsusc.2016.10.010 .
P Ghigna , G Spinolo . High-energy X-ray absorption spectroscopy in materials chemistry . Science of Advanced Materials , 2015 . 7 ( 10 ): 2216 - 2233 . DOI: 10.1166/sam.2015.2270 http://doi.org/10.1166/sam.2015.2270 https://www.researchgate.net/publication/269702545_High-Energy_X-ray_Absorption_Spectroscopy_in_Materials_Chemistry .
A L Ankudinov , B Ravel , J J Rehr , . Real-space multiple-scattering calculation and interpretation of X-ray-absorption near-edge structure . Physical Review B , 1998 . 58 ( 12 ): 7565 - 7576 . DOI: 10.1103/PhysRevB.58.7565 http://doi.org/10.1103/PhysRevB.58.7565 http://cn.bing.com/academic/profile?id=cabbb92644eecabbbbabccb2759e4902&encoded=0&v=paper_preview&mkt=zh-cn .
W Q Shi , L Y Yuan , C Z Wang , . Exploring actinide materials through synchrotron radiation techniques . Advanced Materials , 2014 . 26 ( 46 ): 7807 - 7848 . DOI: 10.1002/adma.201304323 http://doi.org/10.1002/adma.201304323 http://cn.bing.com/academic/profile?id=8cee53d8d0a8cea557d55020d712f6f3&encoded=0&v=paper_preview&mkt=zh-cn .
S Hubert , J Purans , G Heisbourg , . Local structure of actinide dioxide solid solutions Th 1- x U x O 2 and Th 1- x Pu x O 2 . Inorganic Chemistry , 2006 . 45 ( 10 ): 3887 - 3894 . DOI: 10.1021/ic050888y http://doi.org/10.1021/ic050888y http://europepmc.org/abstract/MED/16676947 .
H S Yu , X J Wei , J Li , . The XAFS beamline of SSRF . Nuclear Science and Techniques , 2015 . 26 ( 5 ): 050102 DOI: 10.13538/j.1001-8042/nst.26.050102 http://doi.org/10.13538/j.1001-8042/nst.26.050102 http://cn.bing.com/academic/profile?id=d65d29c13399f2b440cb1f7a854e1b46&encoded=0&v=paper_preview&mkt=zh-cn .
B Ravel , M Newville . Athena, artemis, hephaestus:data analysis for X-ray absorption spectroscopy using IFEFFIT . Journal of Synchrotron Radiation , 2005 . 12 537 - 541 . DOI: 10.1107/S0909049505012719 http://doi.org/10.1107/S0909049505012719 http://cn.bing.com/academic/profile?id=290941795637027eace255d9d09afdb7&encoded=0&v=paper_preview&mkt=zh-cn .
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