Theoretical Insights into Preorganized Pyridylpyrazole-Based Ligands toward the Separation of Am(III)/Eu(III)

doi:10.1021/acs.inorgchem.8b02550

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	Theoretical Insights into Preorganized Pyridylpyrazole-Based Ligands toward the Separation of Am(III)/Eu(III)
	Kong XH(孔祥鹤); Wu QY(吴群燕); Lan JH(蓝建慧); Wang CZ(王聪芝); Chai ZF(柴之芳); Shi WQ(石伟群); Kong, X. H.; Wu, Q. Y.; Lan, J. H.; Wang, C. Z.; Chai, Z. F.; Nie, C. M.; Shi, W. Q.
	2018
发表期刊	INORGANIC CHEMISTRY (IF:4.857[JCR-2016],4.503[5-Year])
ISSN	0020-1669
EISSN	1520-510X
卷号	57 期号:23 页码:14810-14820
文章类型	Article
摘要	Pyridylpyrazole ligands have shown excellent competence for partitioning actinides from lanthanides. As far as we know, the preorganization structure of the ligand has a great impact on the extraction separation ability. However, the mechanism that works well for some ligands but fails for others needs to be clearly elucidated. In this work, we designed three various pyridylpyrazole ligands, BPP, BPBP, and BPPhen, and further preorganized one or both side pyrazole rings of these ligands. The properties of these ligands and the coordination structures, bonding nature and thermodynamic behaviors of the related Am(III) and Eu(III) complexes have been systematically studied in a theoretical fashion. All analyses of geometries, charge transfer, QTAIM (quantum theory of atoms in molecules) and NBO (natural bond orbital) suggest that the Am N bonds possess more covalence compared to that of Eu N bonds. According to the thermodynamic results, increasing the rigidity of the bridging skeleton rather than the side chain can enhance the extraction ability and Am(III)/Eu(III) selectivity of the ligand. This work may identify the reasonability of a useful approach on achieving highly efficient Am(III)/Eu(III) separation through tuning the preorganization level of the ligand and further provide meaningful theoretical basis on the input of preorganization toward ligand design and screening.
DOI	10.1021/acs.inorgchem.8b02550
关键词[WOS]	ENERGY-ADJUSTED PSEUDOPOTENTIALS ; SEGMENTED CONTRACTION SCHEME ; ELECTRONIC-STRUCTURE ; SELECTIVE EXTRACTION ; SOLVENT-EXTRACTION ; COMPLEXES ; ACTINIDE ; DENSITY ; EU(III) ; LANTHANIDE
收录类别	SCI
语种	英语
WOS研究方向	Chemistry
WOS类目	Chemistry, Inorganic & Nuclear
WOS记录号	WOS:000452344400041
引用统计	正在获取...
文献类型	期刊论文
条目标识符	https://ir.ihep.ac.cn/handle/311005/286865
专题	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
第一作者单位	中国科学院高能物理研究所
通讯作者单位	中国科学院高能物理研究所
推荐引用方式 GB/T 7714	Kong XH,Wu QY,Lan JH,et al. Theoretical Insights into Preorganized Pyridylpyrazole-Based Ligands toward the Separation of Am(III)/Eu(III)[J]. INORGANIC CHEMISTRY,2018,57(23):14810-14820.
APA	孔祥鹤.,吴群燕.,蓝建慧.,王聪芝.,柴之芳.,...&Shi, W. Q..(2018).Theoretical Insights into Preorganized Pyridylpyrazole-Based Ligands toward the Separation of Am(III)/Eu(III).INORGANIC CHEMISTRY,57(23),14810-14820.
MLA	孔祥鹤,et al."Theoretical Insights into Preorganized Pyridylpyrazole-Based Ligands toward the Separation of Am(III)/Eu(III)".INORGANIC CHEMISTRY 57.23(2018):14810-14820.