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Density functional theory investigations of the trivalent lanthanide and actinide extraction complexes with diglycolamides
Wang CZ(王聪芝); Lan JH(蓝建慧); Wu QY(吴群燕); Wang, CZ; Lan, JH; Wu, QY; Zhao, YL; Wang, XK; Chai, ZF; Shi, WQ;; Zhao YL(赵宇亮); Chai ZF(柴之芳); Shi WQ(石伟群)
2014
Source PublicationDALTON TRANSACTIONS
ISSN1477-9226
EISSN1477-9234
Volume43Issue:23Pages:8713-8720
AbstractAt present, designing novel ligands for efficient actinide extraction in spent nuclear fuel reprocessing is extremely challenging due to the complicated chemical behaviors of actinides, the similar chemical properties of minor actinides (MA) and lanthanides, and the vulnerability of organic ligands in acidic radioactive solutions. In this work, a quantum chemical study on Am(III), Cm(III) and Eu(III) complexes with N, N,N', N'-tetraoctyl diglycolamide (TODGA) and N, N'-dimethyl-N, N'-diheptyl-3-oxapentanediamide (DMDHOPDA) has been carried out to explore the extraction behaviors of trivalent actinides (An) and lanthanides (Ln) with diglycolamides from acidic media. It has been found that in the 1 : 1 (ligand : metal) and 2 : 1 stoichiometric complexes, the carbonyl oxygen atoms have stronger coordination ability than the ether oxygen atoms, and the interactions between metal cations and organic ligands are substantially ionic. The neutral ML(NO3)(3) (M = Am, Cm, Eu) complexes seem to be the most favorable species in the extraction process, and the predicted relative selectivities are in agreement with experimental results, i.e., the diglycolamide ligands have slightly higher selectivity for Am(III) over Eu(III). Such a thermodynamical priority is probably caused by the higher stabilities of Eu(III) hydration species and Eu(III)-L complexes in aqueous solution compared to their analogues. In addition, our thermodynamic analysis from water to organic medium confirms that DMDHOPDA has higher extraction ability for the trivalent actinides and lanthanides than TODGA, which may be due to the steric hindrance of the bulky alkyl groups of TODGA ligands. This work might provide an insight into understanding the origin of the actinide selectivity and a theoretical basis for designing highly efficient extractants for actinide separation.
Subject AreaChemistry
DOI10.1039/c4dt00032c
Indexed BySCI
Language英语
WOS IDWOS:000336800700017
Citation statistics
Document Type期刊论文
Identifierhttp://ir.ihep.ac.cn/handle/311005/224988
Collection院士
多学科研究中心
Recommended Citation
GB/T 7714
Wang CZ,Lan JH,Wu QY,et al. Density functional theory investigations of the trivalent lanthanide and actinide extraction complexes with diglycolamides[J]. DALTON TRANSACTIONS,2014,43(23):8713-8720.
APA 王聪芝.,蓝建慧.,吴群燕.,Wang, CZ.,Lan, JH.,...&石伟群.(2014).Density functional theory investigations of the trivalent lanthanide and actinide extraction complexes with diglycolamides.DALTON TRANSACTIONS,43(23),8713-8720.
MLA 王聪芝,et al."Density functional theory investigations of the trivalent lanthanide and actinide extraction complexes with diglycolamides".DALTON TRANSACTIONS 43.23(2014):8713-8720.
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