Characterization of redox sensitive plutonium(III) complexed with alkylated 2,6-ditriazinylpyridine (BTP) in organic solution

被引:62
作者
Banik, Nidhu L. [1 ]
Schimmelpfennig, Bernd [1 ]
Marquardt, Christian M. [1 ]
Brendebach, Boris [1 ]
Geist, Andreas [1 ]
Denecke, Melissa A. [1 ]
机构
[1] Karlsruher Inst Technol, Inst Nukl Entsorgung, D-76021 Karlsruhe, Germany
关键词
BASIS-SETS; ABSORPTION-SPECTRA; EU(III); PSEUDOPOTENTIALS; URANIUM(III); EXTRACTION; TRIVALENT; VALENCE; AM(III);
D O I
10.1039/b927016g
中图分类号
O61 [无机化学];
学科分类号
070301 ; 081704 ;
摘要
Spectroscopic, solvent extraction methods and computational chemistry are applied for the characterization of redox sensitive trivalent plutonium complexed with the N-donor extracting agent alkylated 2,6-ditriazinylpyridines (n-C(3)H(7)-BTP) in organic solution. The redox stabilization and speciation of Pu(III) is discussed. Extraction of Pu(III) with n-C3H7-BTP is compared to that for redox stable Am(III). The speciation of Pu(III) with n-C3H7-BTP in organic solution is studied by UV-Vis/NIR and XAFS spectroscopy. Only the 1 : 3 complex, [Pu(n-C(3)H(7)-BTP)(3)](3+) is observed to form, which is confirmed by EXAFS and solvent extraction. The [Pu(n-C(3)H(7)-BTP)(3)](3+) complex is compared to the isostructural U(III), Am(III), and Cm(III) complexes studied earlier.
引用
收藏
页码:5117 / 5122
页数:6
相关论文
共 25 条
[1]   Real-space multiple-scattering calculation and interpretation of x-ray-absorption near-edge structure [J].
Ankudinov, AL ;
Ravel, B ;
Rehr, JJ ;
Conradson, SD .
PHYSICAL REVIEW B, 1998, 58 (12) :7565-7576
[2]  
[Anonymous], 1989, CHEM PHYS LETT, DOI DOI 10.1016/0009-2614(89)85118-8
[3]  
BANIK NL, 2008, ANKA ANGSTROMQUELLE, P145
[4]   DENSITY-FUNCTIONAL EXCHANGE-ENERGY APPROXIMATION WITH CORRECT ASYMPTOTIC-BEHAVIOR [J].
BECKE, AD .
PHYSICAL REVIEW A, 1988, 38 (06) :3098-3100
[5]   X-ray absorption spectroscopic study of trivalent and tetravalent actinides in solution at varying pH values [J].
Brendebach, B. ;
Banik, N. L. ;
Marquardt, Ch. M. ;
Rothe, J. ;
Denecke, M. A. ;
Geckeis, H. .
RADIOCHIMICA ACTA, 2009, 97 (12) :701-708
[6]   Segmented contraction scheme for small-core actinide pseudopotential basis sets [J].
Cao, XY ;
Dolg, M .
JOURNAL OF MOLECULAR STRUCTURE-THEOCHEM, 2004, 673 (1-3) :203-209
[7]   Valence basis sets for relativistic energy-consistent small-core actinide pseudopotentials [J].
Cao, XY ;
Dolg, M ;
Stoll, H .
JOURNAL OF CHEMICAL PHYSICS, 2003, 118 (02) :487-496
[8]   THE ABSORPTION SPECTRA OF PLUTONIUM IONS IN PERCHLORIC ACID SOLUTIONS [J].
COHEN, D .
JOURNAL OF INORGANIC & NUCLEAR CHEMISTRY, 1961, 18 :211-218
[9]   Characterization and comparison of Cm(III) and Eu(III) complexed with 2,6-di(5,6-dipropyl-1,2,4-triazin-3-yl)pyridine using EXAFS, TRFLS, and quantum-chemical methods [J].
Denecke, MA ;
Rossberg, A ;
Panak, PJ ;
Weigl, M ;
Schimmelpfennig, B ;
Geist, A .
INORGANIC CHEMISTRY, 2005, 44 (23) :8418-8425
[10]   A comparative spectroscopic study of U(III)/Am(III) and Ln(III) complexed with N-donor ligands [J].
Denecke, Melissa A. ;
Panak, Petra J. ;
Burdet, Fabien ;
Weigl, Michael ;
Geist, Andreas ;
Klenze, Reinhardt ;
Mazzanti, Marinella ;
Gompper, Klaus .
COMPTES RENDUS CHIMIE, 2007, 10 (10-11) :872-882