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
相关论文
共 49 条
  • [1] Investigation of aquo and chloro complexes of UO22+, NpO2+, Np4+, and Pu3+ by X-ray absorption fine structure spectroscopy
    Allen, PG
    Bucher, JJ
    Shuh, DK
    Edelstein, NM
    Reich, T
    [J]. INORGANIC CHEMISTRY, 1997, 36 (21) : 4676 - 4683
  • [2] Coordination chemistry of trivalent lanthanide and actinide ions in dilute and concentrated chloride solutions
    Allen, PG
    Bucher, JJ
    Shuh, DK
    Edelstein, NM
    Craig, I
    [J]. INORGANIC CHEMISTRY, 2000, 39 (03) : 595 - 601
  • [3] 2ND-ORDER PERTURBATION-THEORY WITH A CASSCF REFERENCE FUNCTION
    ANDERSSON, K
    MALMQVIST, PA
    ROOS, BO
    SADLEJ, AJ
    WOLINSKI, K
    [J]. JOURNAL OF PHYSICAL CHEMISTRY, 1990, 94 (14) : 5483 - 5488
  • [4] Crystal structure diversity in the bis[hydrotris-(3,5-dimethylpyrazolyl)borate]iodouranium(III) complex: from neutral to cationic forms
    Antunes, Maria Augusta
    Santos, Isabel C.
    Bolvin, Helene
    Pereira, Laura C. J.
    Mazzanti, Marinella
    Marcalo, Joaquim
    Almeida, Manuel
    [J]. DALTON TRANSACTIONS, 2013, 42 (24) : 8861 - 8867
  • [5] [An(H2O)9](CF3SO3)3 (An = U-Cm, Cf): Exploring Their Stability, Structural Chemistry, and Magnetic Behavior by Experiment and Theory
    Apostolidis, Christos
    Schimmelpfennig, Bernd
    Magnani, Nicola
    Lindqvist-Reis, Patric
    Walter, Olaf
    Sykora, Richard
    Morgenstern, Alfred
    Colineau, Eric
    Caciuffo, Roberto
    Klenze, Reinhardt
    Haire, Richard G.
    Rebizant, Jean
    Bruchertseifer, Frank
    Fanghaenel, Thomas
    [J]. ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2010, 49 (36) : 6343 - 6347
  • [6] Software News and Update MOLCAS 7: The Next Generation
    Aquilante, Francesco
    De Vico, Luca
    Ferre, Nicolas
    Ghigo, Giovanni
    Malmqvist, Per-Ake
    Neogrady, Pavel
    Pedersen, Thomas Bondo
    Pitonak, Michal
    Reiher, Markus
    Roos, Bjorn O.
    Serrano-Andres, Luis
    Urban, Miroslav
    Veryazov, Valera
    Lindh, Roland
    [J]. JOURNAL OF COMPUTATIONAL CHEMISTRY, 2010, 31 (01) : 224 - 247
  • [7] The influence of radioactive decay on actinide magnetic susceptibility measurements obtained using the Evans method
    Autillo, Matthieu
    Kaden, Peter
    Geist, Andreas
    Guerin, Laetitia
    Moisy, Philippe
    Berthon, Claude
    [J]. PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2014, 16 (18) : 8608 - 8614
  • [8] Gadolinium and neodymium citrates:: Evidence for weak ferromagnetic exchange between gadolinium(III) cations
    Baggio, R
    Calvo, R
    Garland, MT
    Peña, O
    Perec, M
    Rizzi, A
    [J]. INORGANIC CHEMISTRY, 2005, 44 (24) : 8979 - 8987
  • [9] SIMULTANEOUS SIMULATION OF OPTICAL AND MAGNETIC-PROPERTIES OF NEODYMIUM COMPOUNDS
    BEAURY, L
    DEROUET, J
    PORCHER, P
    [J]. JOURNAL OF ALLOYS AND COMPOUNDS, 1995, 225 (1-2) : 28 - 34
  • [10] An alternative approach to the g-matrix: Theory and applications
    Bolvin, Helene
    [J]. CHEMPHYSCHEM, 2006, 7 (07) : 1575 - 1589