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Europium, uranyl, and thorium-phenanthroline amide complexes in acetonitrile solution: an ESI-MS and DFT combined investigation
Xiao CL(肖成梁); Wang CZ(王聪芝); Mei L(梅雷); Zhang XR(张昕蕊); Zhao YL(赵宇亮); Chai ZF(柴之芳); Shi WQ(石伟群); Xiao, CL; Wang, CZ; Mei, L; Zhang, XR; Wall, N; Zhao, YL; Chai, ZF; Shi, WQ
2015
Source PublicationDALTON TRANSACTIONS
ISSN1477-9226
EISSN1477-9234
Volume44Issue:32Pages:14376-14387
Corresponding Author石伟群
SubtypeArticle
AbstractThe tetradentate N,N'-diethyl-N,N'-ditolyl-2,9-diamide-1,10-phenanthroline (Et-Tol-DAPhen) ligand with hard-soft donor atoms has been demonstrated to be promising for the group separation of actinides from highly acidic nuclear wastes. To identify the formed complexes of this ligand with actinides and lanthanides, electrospray ionization mass spectrometry (ESI-MS) combined with density functional theory (DFT) calculations was used to probe the possible complexation processes. The 1 : 2 Eu-L species ([EuL2(NO3)](2+)) can be observed in ESI-MS at low metal-to-ligand ([M]/[L]) ratios, whereas the 1 : 1 Eu-L species ([EuL(NO3)(2)](+)) can be observed when the [M]/[L] ratio is higher than 1.0. However, ([UO2L(NO3)](+)) is the only detected species for the uranyl complexes. The [ThL2(NO3)(2)](2+) species can be observed at low [M]/[L] ratios; the 1 : 2 species ([ThL2(NO3)](3+)) and a new 1 : 1 species ([ThL(NO3)(3)](+)) can be detected at high [M]/[L] ratios. Collision-induced dissociation (CID) results showed that Et-Tol-DAPhen ligands can coordinate strongly with metal ions, and the coordination moieties remain intact under CID conditions. Natural bond orbital (NBO), molecular electrostatic potential (MEP), electron localization function (ELF), atoms in molecules (AIM) and molecular orbital (MO) analyses indicated that the metal-ligand bonds of the actinide complexes exhibited more covalent character than those of the lanthanide complexes. In addition, according to thermodynamic analysis, the stable cationic M-L complexes in acetonitrile are found to be in good agreement with the ESI-MS results.
Subject AreaChemistry
DOI10.1039/c5dt01766a
Indexed BySCI ; EI
Language英语
WOS Research AreaChemistry, Inorganic & Nuclear
WOS SubjectChemistry
WOS IDWOS:000359088200026
Citation statistics
Document Type期刊论文
Identifierhttp://ir.ihep.ac.cn/handle/311005/228692
Collection院士
多学科研究中心
Recommended Citation
GB/T 7714
Xiao CL,Wang CZ,Mei L,et al. Europium, uranyl, and thorium-phenanthroline amide complexes in acetonitrile solution: an ESI-MS and DFT combined investigation[J]. DALTON TRANSACTIONS,2015,44(32):14376-14387.
APA 肖成梁.,王聪芝.,梅雷.,张昕蕊.,赵宇亮.,...&Shi, WQ.(2015).Europium, uranyl, and thorium-phenanthroline amide complexes in acetonitrile solution: an ESI-MS and DFT combined investigation.DALTON TRANSACTIONS,44(32),14376-14387.
MLA 肖成梁,et al."Europium, uranyl, and thorium-phenanthroline amide complexes in acetonitrile solution: an ESI-MS and DFT combined investigation".DALTON TRANSACTIONS 44.32(2015):14376-14387.
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