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Ligand-exchange mechanism: new insight into solid-phase extraction of uranium based on a combined experimental and theoretical study
Tian, Y; Fu, J; Zhang, Y; Cao, KC; Bai, CY; Wang, DQ; Li, SJ; Xue, Y; Ma, LL; Zheng, C; Wang DQ(王东琪)
2015
发表期刊PHYSICAL CHEMISTRY CHEMICAL PHYSICS
卷号17期号:11页码:7214-7223
文章类型Article
摘要In numerous reports on selective solid-phase extraction (SPE) of uranium, the extraction of uranium is generally accepted as a direct coordination of the ligands on the solid matrix with the uranyl, in which the critical effect of the hydration shell on the uranyl is neglected. The related mechanism in the extraction process remains unclear. Herein, the detailed calculation of activation energy and the geometry of the identified transition states reveal that the uranium extraction by a newly-synthesized urea-functionalized graphite oxide (Urea-GO) is in essence an exchange process between the ligands on Urea-GO and the coordinated water molecules in the first hydration shell of the uranyl. Moreover, we demonstrate that it is the ketone oxygen in the urea ligand to displace the coordinated water molecule of uranyl due to its stronger bonding ability and lower steric-hindrance, whereas the nitrogen atom in the same ligand is proved to be an electron donor that enables the oxygen atom to have stronger affinity for uranium through electron delocalization effects evaluated on the basis of calculations of the second-order interaction energy between donor and acceptor orbitals. We therefore propose a new ligand-exchange mechanism for the SPE process. This study advances the fundamental understanding of uranium extraction, and provides theoretical and practical guidance on ligand design for selective complexation of uranium(VI) and other metal ions in aqueous solution. Finally, the effect of nitrate ions on the extraction of uranyl was successfully explained based on the experimental and theoretical study.
学科领域Chemistry; Physics
DOI10.1039/c4cp05508j
收录类别SCI
WOS类目Chemistry, Physical ; Physics, Atomic, Molecular & Chemical
WOS记录号WOS:000351436400015
引用统计
被引频次:14[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/311005/228279
专题多学科研究中心
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GB/T 7714
Tian, Y,Fu, J,Zhang, Y,et al. Ligand-exchange mechanism: new insight into solid-phase extraction of uranium based on a combined experimental and theoretical study[J]. PHYSICAL CHEMISTRY CHEMICAL PHYSICS,2015,17(11):7214-7223.
APA Tian, Y.,Fu, J.,Zhang, Y.,Cao, KC.,Bai, CY.,...&王东琪.(2015).Ligand-exchange mechanism: new insight into solid-phase extraction of uranium based on a combined experimental and theoretical study.PHYSICAL CHEMISTRY CHEMICAL PHYSICS,17(11),7214-7223.
MLA Tian, Y,et al."Ligand-exchange mechanism: new insight into solid-phase extraction of uranium based on a combined experimental and theoretical study".PHYSICAL CHEMISTRY CHEMICAL PHYSICS 17.11(2015):7214-7223.
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