Complexation of vanadium with amidoxime and carboxyl groups: uncovering the competitive role of vanadium in uranium extraction from seawater

doi:10.1515/ract-2016-2713

CORC > 上海应用物理研究所 > 中国科学院上海应用物理研究所 > 中科院上海应用物理研究所2011-2017年

	Complexation of vanadium with amidoxime and carboxyl groups: uncovering the competitive role of vanadium in uranium extraction from seawater
	Wang, CZ; Wu, QY; Lan, JH; Chai, ZF; Wu, GZ; Shi, WQ
刊名	RADIOCHIMICA ACTA
	2017
卷号	105 期号:7 页码:541-553
关键词	Molecular-energies m(Co)(6) M=cr Ab-initio Density Uranyl Adsorption Recovery Adsorbents Stability Ions
ISSN号	0033-8230
DOI	10.1515/ract-2016-2713
文献子类	期刊论文
英文摘要	At present, amidoxime-based adsorbents are considered to be the most promising materials for extraction of uranium from seawater. However, the high concentrations of transition metals especially vanadium strongly compete with uranium in the sequestration process, which is extremely limited the commercial use of amidoxime-based adsorbents. In this work, the coordination modes, bonding nature, and stabilities of possible vanadium(IV) (VO2+) and (V) (VO2+, VO3+, V5+) complexes with amidoximate (AO(-)), carboxyl (Ac-), glutarimidedioximate (HA(-)) and deprotonated glutarimidedioximate (A(2-)) on single and double alkyl chains (R = C-13 H-26) are systematically explored by quantum chemical calculations. Different from the uranyl (UO22+) complexes, the AO - groups of the vanadium(IV) and (V) complexes prefer to coordinate as monodentate and chelate ligands, while few species with AO - groups in eta(2)-binding mode have been observed in the vanadium complexes. Besides, the vanadium complexes are predicted to have obvious covalent metal-ligand bonds. According to thermodynamic stability analysis, all the vanadium complexes with AO(-), Ac-, HA(-) and A(2-) ligands on double alkyl chains are found to be more stable than corresponding complexes with ligands on a single chain. The synergistic effect of the amidoxime and carboxyl groups can be observed in most of VO2+ and VO3+ complexes with mixed ligands (AO(-)/Ac-). The vanadium(IV) and (V) complexes are more stable than the corresponding uranyl complexes, and the adsorption capability of the amidoxime-based adsorbents toward vanadium(V) ions decrease in the order of VO2+ > VO3+ > V5+. The dioxovanadium cation VO2+ is predicted to form multinuclear vanadium complex in the sequestration process, possibly resulting in higher stable VO2+ complexes. Therefore, the higher complexation ability of the amidoxime-based adsorbents toward vanadium over uranium is probably due to the differences in the coordination modes and bonding nature. The current results might provide important clues for rational design of efficient ligands in sequestration of uranium from seawater.
WOS关键词	MOLECULAR-ENERGIES ; M(CO)(6) M=CR ; AB-INITIO ; DENSITY ; URANYL ; ADSORPTION ; RECOVERY ; ADSORBENTS ; STABILITY ; IONS
语种	英语
WOS记录号	WOS:000405324600004
内容类型	期刊论文
源URL	[http://ir.sinap.ac.cn/handle/331007/28586]
专题	上海应用物理研究所_中科院上海应用物理研究所2011-2017年
推荐引用方式 GB/T 7714	Wang, CZ,Wu, QY,Lan, JH,et al. Complexation of vanadium with amidoxime and carboxyl groups: uncovering the competitive role of vanadium in uranium extraction from seawater[J]. RADIOCHIMICA ACTA,2017,105(7):541-553.
APA	Wang, CZ,Wu, QY,Lan, JH,Chai, ZF,Wu, GZ,&Shi, WQ.(2017).Complexation of vanadium with amidoxime and carboxyl groups: uncovering the competitive role of vanadium in uranium extraction from seawater.RADIOCHIMICA ACTA,105(7),541-553.
MLA	Wang, CZ,et al."Complexation of vanadium with amidoxime and carboxyl groups: uncovering the competitive role of vanadium in uranium extraction from seawater".RADIOCHIMICA ACTA 105.7(2017):541-553.