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A density functional theory study on the interaction between UO22+ and the carbamoylphosphoramidic acid ligand for uranium extraction from seawater
Guo, XJ; Li, C; Hu, JT; Ma, HJ; Qian, HL
2018
Source PublicationNUCLEAR SCIENCE AND TECHNIQUES
ISSN1001-8042
Volume29Issue:6Pages:-
Subtype期刊论文
AbstractPhosphorylurea molecules, which contain both phosphoryl and carbonyl groups, are considered efficient extractants for UO22+. This study aims to explain the complexation of UO22+ with carbamoylphosphoramidic acid (CPO), a simple model for phosphorylurea, for ligand design for uranium recovery from seawater using density functional theory calculations, natural bond order analysis, and the quantum theory of atoms in molecules. The results showed that, when CPO acts as a monodentate ligand, the affinity of phosphoryl for UO22+ is stronger than that of carbonyl, and CPO coordinates with UO22+ through the phosphoryl oxygen atom. When CPO serves as a bidentate ligand, both the phosphoryl and carbonyl oxygen atoms connect to UO22+, and the U-O(carbonyl) bond plays a more important role than the U-O(phosphoryl) bond in the interaction between UO22+ and CPO. This paradox may be caused by the significant charge transfer from the U- O(carbonyl) pi bond orbital to the C-N sigma antibond orbital of the bidentate CPO. The NH spacer between the phosphoryl and carbonyl groups could ensure the delocalization of the electron system of the molecule. The bidentate binding motif is favored by entropy and opposed by enthalpy, while the monodentate binding motif is favored by enthalpy and opposed by entropy. Ultimately, the bidentate binding motif is more favorable than the monodentate one. As expected, the interaction between UO22+ and the deprotonated CPO is stronger than that between UO22+ and the neutral CPO. Comparing the interaction between UO22+ and CPO with that between UO22+ and N-phenylcarbamoylphosphoramidic acid (PhCPO), formed by replacing one hydrogen atom from the terminal nitrogen atom of CPO with a phenyl group, the phenyl substituent at the terminal nitrogen atom of PhCPO shows a slightly negative effect on the interaction between UO22+ and PhCPO.
KeywordAb-initio Pseudopotentials Sequestering Uranium Dft Investigations Parameter Sets Uranyl-ion Energy Complexes Actinides Potentials Solvation
DOI10.1007/s41365-018-0422-0
Indexed BySCI
Language英语
WOS IDWOS:000433263900014
Citation statistics
Cited Times:1[WOS]   [WOS Record]     [Related Records in WOS]
Document Type期刊论文
Identifierhttp://ir.sinap.ac.cn/handle/331007/28903
Collection中科院上海应用物理研究所2011-2020年
Affiliation1.Guo, XJ
2.Li, C
3.Hu, JT
4.Ma, HJ
5.Qian, HL
Recommended Citation
GB/T 7714
Guo, XJ,Li, C,Hu, JT,et al. A density functional theory study on the interaction between UO22+ and the carbamoylphosphoramidic acid ligand for uranium extraction from seawater[J]. NUCLEAR SCIENCE AND TECHNIQUES,2018,29(6):-.
APA Guo, XJ,Li, C,Hu, JT,Ma, HJ,&Qian, HL.(2018).A density functional theory study on the interaction between UO22+ and the carbamoylphosphoramidic acid ligand for uranium extraction from seawater.NUCLEAR SCIENCE AND TECHNIQUES,29(6),-.
MLA Guo, XJ,et al."A density functional theory study on the interaction between UO22+ and the carbamoylphosphoramidic acid ligand for uranium extraction from seawater".NUCLEAR SCIENCE AND TECHNIQUES 29.6(2018):-.
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