中国科学院机构知识库网格
Chinese Academy of Sciences Institutional Repositories Grid
Density functional theory investigations of the trivalent lanthanide and actinide extraction complexes with diglycolamides

文献类型:期刊论文

作者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;
刊名DALTON TRANSACTIONS
出版日期2014
卷号43期号:23页码:8713-8720
英文摘要At 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.
学科主题Chemistry
收录类别SCI
WOS记录号WOS:000336800700017
公开日期2016-05-03
源URL[http://ir.ihep.ac.cn/handle/311005/224988]  
专题高能物理研究所_院士
高能物理研究所_多学科研究中心
推荐引用方式
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.

入库方式: OAI收割

来源:高能物理研究所

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