Theoretical studies on the synergistic extraction of Am3+ and Eu3+ with CMPO-HDEHP and CMPO-HEH[EHP] systems

doi:10.1039/c8dt00134k

	Theoretical studies on the synergistic extraction of Am3+ and Eu3+ with CMPO-HDEHP and CMPO-HEH[EHP] systems
	Chai, ZF; Song, G; Lan, JH; Wu, QY; Wang, CZ; Huang, PW; Shi WQ(石伟群); Chai ZF(柴之芳); Lan JH(蓝建慧); Wu QY(吴群燕)
刊名	DALTON TRANSACTIONS
	2018
卷号	47 期号:15 页码:5474-5482
ISSN号	1477-9226
DOI	10.1039/c8dt00134k
文献子类	Article
英文摘要	In recent years, there has been a trend to use synergistic systems of neutral and acidic extractants into a single-solvent formulation to achieve Ln(3+)/An(3+) extraction and separation via simplified processing schemes. In this study, geometrical structures, bonding nature, and thermodynamic stabilities of a series of possible extraction complexes of Am3+ and Eu3+ with two neutral-acid synergistic systems (CMPO-HDEHP and CMPO-HEH[EHP]) were theoretically studied using scalar-relativistic density functional theory (DFT). It is found that hydrogen bonds between neutral and acid ligands may greatly influence the Eu3+/Am3+ extraction and separation performance of the two synergistic systems. According to natural bond orbital (NBO) and energy decomposition analyses (EDA), the phosphoryl oxygen atoms of HDEHP or HEH[EHP] have higher affinity for Eu3+ and Am3+ than those of the CMPO ligand. Since weak but different extents of covalency exist in Eu- and Am-complexes, Eu3+/Am3+ separation via these two systems may be attributed to the different compositions of interactions between the metal ions and ligands. Thermodynamic analysis shows that the neutral complexes ML(NO3)(2) (M = Eu and Am; L = [CMPO-DEHP](-) and [CMPO-EH[EHP]](-)) appear to be the most probable species in the complexation process.
电子版国际标准刊号	1477-9234
WOS关键词	SEPARATING TRIVALENT LANTHANIDES ; SOLVENT-EXTRACTION ; TRANSURANIC ELEMENTS ; COMPLEXATION THERMODYNAMICS ; CORRELATION-ENERGY ; COMBINING CMPO ; LIGANDS ; DENSITY ; ACTINIDES ; PSEUDOPOTENTIALS
WOS研究方向	Chemistry
语种	英语
WOS记录号	WOS:000430328100042
内容类型	期刊论文
源URL	[http://ir.ihep.ac.cn/handle/311005/285869]
专题	高能物理研究所_多学科研究中心
通讯作者	Shi WQ(石伟群)
作者单位	中国科学院高能物理研究所
推荐引用方式 GB/T 7714	Chai, ZF,Song, G,Lan, JH,et al. Theoretical studies on the synergistic extraction of Am3+ and Eu3+ with CMPO-HDEHP and CMPO-HEH[EHP] systems[J]. DALTON TRANSACTIONS,2018,47(15):5474-5482.
APA	Chai, ZF.,Song, G.,Lan, JH.,Wu, QY.,Wang, CZ.,...&Shi, WQ.(2018).Theoretical studies on the synergistic extraction of Am3+ and Eu3+ with CMPO-HDEHP and CMPO-HEH[EHP] systems.DALTON TRANSACTIONS,47(15),5474-5482.
MLA	Chai, ZF,et al."Theoretical studies on the synergistic extraction of Am3+ and Eu3+ with CMPO-HDEHP and CMPO-HEH[EHP] systems".DALTON TRANSACTIONS 47.15(2018):5474-5482.