Magnetic susceptibility of actinide(III) cations: an experimental and theoretical study

被引:18
作者
Autillo, Matthieu [1 ]
Guerin, Laetitia [1 ]
Bolvin, Helene [2 ]
Moisy, Philippe [1 ]
Berthon, Claude [1 ]
机构
[1] CEA, DRCP, RadioChem & Proc Dept, Nucl Energy Div, BP 17171, F-30207 Bagnols Sur Ceze, France
[2] Univ Toulouse 3, Lab Phys & Chim Quant, 118 Route Narbonne, F-31062 Toulouse, France
关键词
AQUEOUS-SOLUTIONS; RADIATION CHEMISTRY; HYDROGEN-PEROXIDE; BASIS-SETS; RADIOLYSIS; TRIVALENT; NEODYMIUM; SPECTRA; IONS; WATER;
D O I
10.1039/c5cp07456h
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
In a previous paper, the influence of radioactive decay (alpha and beta(-)) on magnetic susceptibility measurements by the Evans method has been demonstrated by the study of two americium isotopes. To characterize more accurately this phenomenon and particularly its influence on the Curie law, a new study has been performed on two uranium isotopes (U-238 and U-233) and on tritiated water ((H2O)-H-3). The results on the influence of alpha emissions have established a relationship between changes in the temperature dependence and the radioactivity in solution. Regarding the beta(-) emissions, less influence was observed while no temperature dependence linked to this kind of radioactive emission could be identified. Once magnetic susceptibility measurements of actinide(III) cations were corrected from radioactivity effects, methods of quantum chemistry have been used on free ions and aquo complexes to calculate the electronic structure explaining the magnetic properties of Pu(III), Am(III) and Cm(III). The ligand field effect on the magnetic behavior (the Curie constant and temperature-independent susceptibilities) was analyzed by considering different solvation environments.
引用
收藏
页码:6515 / 6525
页数:11
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