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Selective Extraction of Americium(III) over Europium(III) with the Pyridylpyrazole Based Tetradentate Ligands: Experimental and Theoretical Study
Wang; JR; Su; DP; Wang DQ(王东琪); Wang; DQ; Ding; SD; Huang; C; Huang; H; Hu; XY; Wang; ZP; Li; SM
2015
发表期刊INORGANIC CHEMISTRY
卷号54期号:22页码:10648-10655
摘要1,3-Bis[3-(2-pyridyl)pyrazol-1-yl]propane (Bippp) and 1,2-bis[3-(2-pyridyl)pyrazy1-1-methyl]benzene (Dbnpp), the pyridylpyrazole based tetradentate ligands, were synthesized and characterized by MS, NMR, and FT-IR The solvent extraction and complexation behaviors of Am(III) and Eu(III) with the ligands were investigated experimentally and theoretically. In the presence of 2-bromohexanoic acid, the two ligands can effectively extract Am(III) over Eu(III) and other rare earth(III) metals (RE(III)) in HNO3 solution with the separation factors (SFAm/RE) ranging from 15 to 60. Slope analyses showed that both Am(III) and Eu(III) were extracted as monosolvated species, which agrees well with the results observed from X-ray crystallography and MS analyses. The stability constants (log K) obtained from UV-vis titration for Eu(III) complexes with Bippp and Dbnpp are 4.75 +/- 0.03 and 4.45 +/- 0.04, respectively. Both UV-vis titration and solvent extraction studies indicated that Bippp had stronger affinity for Eu(III) than Dbnpp, which is confirmed by density functional theory (DFT) calculations. DFT calculations revealed that the AmL(NO3)(3) (L = Bippp and Dbnpp) complexes are thermodynamically more stable in water than their Eu(III) analogues, which is caused by greater covalency of the Am-N than Eu-N bonds. Theoretical studies gave an insight into the nature of the M(II)-ligand bonding interactions.
文章类型Article
学科领域Chemistry
DOI10.1021/acs.inorgchem.5b01452
收录类别SCI
WOS类目Chemistry, Inorganic & Nuclear
WOS记录号WOS:000364981300019
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被引频次:8[WOS]   [WOS记录]     [WOS相关记录]
文献类型期刊论文
条目标识符http://ir.ihep.ac.cn/handle/311005/229069
专题多学科研究中心
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Wang,JR,Su,et al. Selective Extraction of Americium(III) over Europium(III) with the Pyridylpyrazole Based Tetradentate Ligands: Experimental and Theoretical Study[J]. INORGANIC CHEMISTRY,2015,54(22):10648-10655.
APA Wang.,JR.,Su.,DP.,王东琪.,...&SM.(2015).Selective Extraction of Americium(III) over Europium(III) with the Pyridylpyrazole Based Tetradentate Ligands: Experimental and Theoretical Study.INORGANIC CHEMISTRY,54(22),10648-10655.
MLA Wang,et al."Selective Extraction of Americium(III) over Europium(III) with the Pyridylpyrazole Based Tetradentate Ligands: Experimental and Theoretical Study".INORGANIC CHEMISTRY 54.22(2015):10648-10655.
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