CAS OpenIR  > 中科院上海应用物理研究所2011-2019年
Theoretical studies on the complexation of uranyl with typical carboxylate and amidoximate ligands
Xu ChaoFei; Su Jing; Xu Xiang; Li Jun
2013
Source PublicationSCIENCE CHINA-CHEMISTRY
ISSN1674-7291; 1869-1870
Volume56Issue:11Pages:CONCATENATE(Sheet1!I369,-Sheet1!J369)
AbstractUnderstanding of the bonding nature of uranyl and various ligands is the key for designing robust sequestering agents for uranium extraction from seawater. In this paper thermodynamic properties related to the complexation reaction of uranyl(VI) in aqueous solution (i.e. existing in the form of UO2(H2O)(5) (2+)) by several typical ligands (L) including acetate (CH3CO2 (-)), bicarbonate (HOCO2 (-)), carbonate (CO3 (2-)), CH3(NH2)CNO- (acetamidoximate, AO(-)) and glutarimidedioximate (denoted as GDO(2-)) have been investigated by using relativistic density functional theory (DFT). The geometries, vibrational frequencies, natural net charges, and bond orders of the formed uranyl-L complexes in aqueous solution are studied. Based on the DFT analysis we show that the binding interaction between uranyl and amidoximate ligand is the strongest among the selected complexes. The thermodynamics of the complexation reaction are examined, and the calculated results show that complexation of uranyl with amidoximate ligands is most preferred thermodynamically. Besides, reaction paths of the substitution complexation of solvated uranyl by acetate and AO(-) have been studied, respectively. We have obtained two minima along the reaction path of solvated uranyl with acetate, the monodentate-acetate complex and the bidentate-acetate one, while only one minimum involving monodentate-AO complex has been located for AO(-) ligand. Comparing the energy barriers of the two reaction paths, we find that complexation of uranyl with AO(-) is more difficult in kinetics, though it is more preferable in thermodynamics. These results show that theoretical studies can help to select efficient ligands with fine-tuned thermodynamic and kinetic properties for binding uranyl in seawater.
Indexed BySCI
Language英语
Funding Project应物所项目组
WOS IDWOS:000326327500006
Citation statistics
Cited Times:15[WOS]   [WOS Record]     [Related Records in WOS]
Document Type期刊论文
Identifierhttp://ir.sinap.ac.cn/handle/331007/13963
Collection中科院上海应用物理研究所2011-2019年
Recommended Citation
GB/T 7714
Xu ChaoFei,Su Jing,Xu Xiang,et al. Theoretical studies on the complexation of uranyl with typical carboxylate and amidoximate ligands[J]. SCIENCE CHINA-CHEMISTRY,2013,56(11):CONCATENATE(Sheet1!I369,-Sheet1!J369).
APA Xu ChaoFei,Su Jing,Xu Xiang,&Li Jun.(2013).Theoretical studies on the complexation of uranyl with typical carboxylate and amidoximate ligands.SCIENCE CHINA-CHEMISTRY,56(11),CONCATENATE(Sheet1!I369,-Sheet1!J369).
MLA Xu ChaoFei,et al."Theoretical studies on the complexation of uranyl with typical carboxylate and amidoximate ligands".SCIENCE CHINA-CHEMISTRY 56.11(2013):CONCATENATE(Sheet1!I369,-Sheet1!J369).
Files in This Item:
File Name/Size DocType Version Access License
Theoretical studies (665KB) 开放获取CC BY-NC-SAView Application Full Text
Related Services
Recommend this item
Bookmark
Usage statistics
Export to Endnote
Google Scholar
Similar articles in Google Scholar
[Xu ChaoFei]'s Articles
[Su Jing]'s Articles
[Xu Xiang]'s Articles
Baidu academic
Similar articles in Baidu academic
[Xu ChaoFei]'s Articles
[Su Jing]'s Articles
[Xu Xiang]'s Articles
Bing Scholar
Similar articles in Bing Scholar
[Xu ChaoFei]'s Articles
[Su Jing]'s Articles
[Xu Xiang]'s Articles
Terms of Use
No data!
Social Bookmark/Share
File name: Theoretical studies on the complexation of uranyl with typical carboxylate and amidoximate ligands.pdf
Format: Adobe PDF
All comments (0)
No comment.
 

Items in the repository are protected by copyright, with all rights reserved, unless otherwise indicated.