Europium, uranyl, and thorium-phenanthroline amide complexes in acetonitrile solution: an ESI-MS and DFT combined investigation
文献类型：期刊论文
| 作者 | 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
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| 刊名 | DALTON TRANSACTIONS
 |
| 出版日期 | 2015 |
| 卷号 | 44期号:32页码:14376-14387 |
| 通讯作者 | 石伟群 |
| 英文摘要 | The 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. |
| 学科主题 | Chemistry |
| 类目[WOS] | Chemistry, Inorganic & Nuclear |
| 收录类别 | SCI ; EI |
| WOS记录号 | WOS:000359088200026 |
| 公开日期 | 2016-05-03 |
| 源URL | [http://ir.ihep.ac.cn/handle/311005/228692]  |
| 专题 | 高能物理研究所_院士 高能物理研究所_多学科研究中心 |
| 推荐引用方式 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. |
入库方式： OAI收割
来源：高能物理研究所
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