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Influence of a Bridging Group and the Substitution Effect of Bis(1,2,4-triazine) N-Donor Extractants on Their Interactions with a Np-V Cation
Yang X(杨霞); Liang YN(梁艳妮); Yang, X; Liang, YN; Ding, SD; Li, SJ; Chai, ZF; Wang, DQ; Chai ZF(柴之芳); Wang DQ(王东琪)
刊名INORGANIC CHEMISTRY
2014
卷号53期号:15页码:7848-7860
学科分类Chemistry
DOI10.1021/ic500138w
英文摘要The present theoretical study provides a realistic bonding characteristics of a variety of neptunyl complexes evaluation of the equilibrium structure, reaction modes, and formed with bis(triazinyl) N-donor extractants, which differ in their bridging groups such as pyridine, bipyridines, and orthophenanthroline, corresponding to the ligands (L) of tridentate bis(triazinyl)pyridines and tetradentate bis(triazinyl)-bipyridines and bis(triazinyl)-1,10-phenanthrolines (BTPhens), respectively. Our calculations show that coordination of [NpO2](+) to tetradentate ligands is more favorable than that to tridentate ones no matter in a gas, aqueous, or organic phase. The presence of nitrate ions can enhance the coordination ability of neptunyl and stabilize the neutral NpO2L(NO3) complexes in thermodynamics. Our studies indicate that the complexation reaction mode [NpO2(H2O)(n)](+) + L + NO3-) NpO2L(NO3) + nH(2)O is the most probable at the interface between water and the organic phase. The contribution of an orthophenanthroline bridging group is relatively more pronounced compared to its pyridine counterpart in ligand-exchange reaction. Complexation reactions of hydrated neptunyl with C2-BTPhen and BTPhen assisted by a nitrate ion are favorable thermodynamically, resulting from the least deformation of the ligand and strong complexation stability. The quantum theory of atoms-in-molecules and charge decomposition analysis suggest that electron delocalization and charge transfer are the main reasons responsible for stabilization of the tetradentate complexes and reveal a strong ionic feature of the Np-ligand bonds. Inspection of the frontier molecular orbitals reveals a distinct Sf orbital (Np) interaction with ligand atoms, implying the extent of f-based covalenc-y. Our study may facilitate the rational design of ligands toward the improvement of their binding ability with Np-V and more efficient separation of Np in spent nuclear fuels.
收录类别SCI
WOS记录号WOS:000339982400010
引用统计
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/311005/225034
专题院士_期刊论文
中国科学院高能物理研究所_多学科研究中心
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GB/T 7714
Yang X,Liang YN,Yang, X,et al. Influence of a Bridging Group and the Substitution Effect of Bis(1,2,4-triazine) N-Donor Extractants on Their Interactions with a Np-V Cation[J]. INORGANIC CHEMISTRY,2014,53(15):7848-7860.
APA 杨霞.,梁艳妮.,Yang, X.,Liang, YN.,Ding, SD.,...&王东琪.(2014).Influence of a Bridging Group and the Substitution Effect of Bis(1,2,4-triazine) N-Donor Extractants on Their Interactions with a Np-V Cation.INORGANIC CHEMISTRY,53(15),7848-7860.
MLA 杨霞,et al."Influence of a Bridging Group and the Substitution Effect of Bis(1,2,4-triazine) N-Donor Extractants on Their Interactions with a Np-V Cation".INORGANIC CHEMISTRY 53.15(2014):7848-7860.
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