Structural Properties and Charge Distribution of the Sodium Uranium, Neptunium, and Plutonium Ternary Oxides: A Combined X-ray Diffraction and XANES Study

被引:19
作者
Smith, Anna L. [1 ,2 ,5 ]
Martin, Philippe [3 ]
Prieur, Damien [1 ]
Scheinost, Andreas C. [4 ]
Raison, Philippe E. [1 ]
Cheetharn, Anthony K. [2 ]
Konings, Rudy J. M. [1 ]
机构
[1] Commiss European Communities, Inst Transuranium Elements ITU, JRC, POB 2340, D-76125 Karlsruhe, Germany
[2] Univ Cambridge, Dept Mat Sci & Met, 27 Charles Babbage Rd, Cambridge CB3 0FS, England
[3] CEN Cadarache, DEC, DEN, CEA, F-13108 St Paul Les Durance, France
[4] HZDR, Inst Resource Ecol, POB 10119, D-01314 Dresden, Germany
[5] Delft Univ Technol, Radiat Sci & Technol Dept, NERA, Mekelweg 15, NL-2629 JB Delft, Netherlands
关键词
CRYSTAL-STRUCTURE; MAGNETIC-PROPERTIES; LIQUID-SODIUM; ABSORPTION; NA; TRANSMUTATION; SPECTROSCOPY; OXIDATION; NP(VII); NA4UO5;
D O I
10.1021/acs.inorgchem.5b02476
中图分类号
O61 [无机化学];
学科分类号
070301 ; 081704 ;
摘要
The charge distributions in alpha-Na2UO4, Na3NpO4, alpha-Na2NpO4, Na4NpO5, Na5NpO6, Na2PuO3, Na4PuO5, and Na5PuO6 are investigated in this work using X-ray absorption near-edge structure (XANES) spectroscopy at the U-L-3, Np-L-3, and Pu-L-3 edges. In addition, a Rietveld refinement of monoclinic Na2PuO3, in space group C2/c, is reported for the first time, and the existence of the isostructural Na2NpO3 phase is revealed. In contrast to measurements in solution, the number of published XANES data for neptunium and plutonium solid phases with a valence state higher than IV is very limited. The present results cover a wide range of oxidation states, namely, IV to VII, and can serve as reference for future investigations. The sodium actinide series show a variety of local coordination geometries, and correlations between the shape of the XANES spectra and the local structural environments are discussed herein.
引用
收藏
页码:1569 / 1579
页数:11
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