Complexation behavior of Eu(III), Tb(III), Tm(III), and Am(III) with three 1,10-phenanthroline-type ligands: insights from density functional theory

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• 作者：Yanqiu Yang ; Yu Fang ; Jun Liu ; Shiyuan Hu ; Sheng Hu…
• 关键词：Density functional theory ; Second ; order Møller–Plesset perturbation theory ; Computational study ; Selective extraction ; Natural bond orbital analysis
• 刊名：Journal of Molecular Modeling
• 出版年：2015
• 出版时间：July 2015
• 年：2015
• 卷：21
• 期：7
• 全文大小：3,273 KB
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• 作者单位：Yanqiu Yang (1)
  Yu Fang (2)
  Jun Liu (1)
  Shiyuan Hu (2)
  Sheng Hu (1)
  Liang Yang (1)
  Dawei Wang (2)
  Huabei Zhang (2)
  Shunzhong Luo (1)
  
  1. Institute of Nuclear Physics and Chemistry, China Academy of Engineering Physics, Mianyang, Sichuan, 621900, China
  2. Key Laboratory of Radiopharmaceuticals of Ministry of Education, College of Chemistry, Beijing Normal University, Beijing, 100875, China
  
• 刊物类别：Chemistry and Materials Science
• 刊物主题：Chemistry
  Computer Applications in Chemistry
  Biomedicine
  Molecular Medicine
  Health Informatics and Administration
  Life Sciences
  Computer Application in Life Sciences
  
• 出版者：Springer Berlin / Heidelberg
• ISSN：0948-5023

文摘

Extraction complexes of Eu(III), Tb(III), Tm(III), and Am(III) with three 1,10-phenanthroline-type ligands have been studied, primarily using density functional theory (DFT). The same accuracies and optimized structural geometries were obtained whether optimization of the [ML₂(NO₃)]2+ complexes was performed at the B3LYP/6-31G(d)/RECP or the MP2/6-31G(d)/RECP level of theory. Calculations carried out at the B3LYP/6-311G(d, p)/RECP level of theory indicated that solvation does not favor the formation of these complexes. Moreover, the ΔG _g and ΔG _solv values for the reactions leading to the formation of [LnL₂(NO₃)]2+ complexes were seen to decrease with increasing atomic number of the lanthanide (from Eu to Tb to Tm). In addition, when a strongly hydrophobic benzo[e][1,2,4]triazine group was created in each ligand, ligand selectivity for actinides/lanthanides in acidic media improved. Even greater ligand selectivity for actinides/lanthanides in acidic media was obtained when a 5,6-diphenyl-1,2,4-triazine group was created in each ligand instead of a benzo[e][1,2,4]triazine group. Vibrational analysis and NMR spectroscopic analysis were also performed on all of the studied ligands and the metal complexes that included them. Further in-depth investigations should be undertaken in this field.