Citation: BI Yan-Ting, YAO Jun, SHEN Zhong-Hui, ZHANG Hong-Xing, PAN Qing-Jiang. Interaction Behavior Between Hexa-dentate Polypyrrolic Macrocycles and Actinyl Species: Bonding, Thermodynamic and Spectroscopic Properties[J]. Chinese Journal of Inorganic Chemistry, ;2018, 34(6): 1071-1078. doi: 10.11862/CJIC.2018.136 shu

Interaction Behavior Between Hexa-dentate Polypyrrolic Macrocycles and Actinyl Species: Bonding, Thermodynamic and Spectroscopic Properties

1.
Science and Technology Division, School of Chemistry and Materials Science, Heilongjiang University, Harbin 150080, China
2.
Institute of Theoretical Chemistry, Jilin University, Changchun 130023, China

Corresponding author: SHEN Zhong-Hui, shenzhonghui@hlju.edu.cn PAN Qing-Jiang, panqjitc@163.com
Received Date: 7 January 2018
Revised Date: 20 March 2018

Figures(4)

A relativistic density functional theory (DFT) was used to systematically examine a series of uranyl and transuranyl complexes of N-donor macrocyclic ligands, [(AnO₂)(Ln)]^2-(labeled as nAn; n=1~3; An=U, Np and Pu). Further comparison was made with[(UO₂)(L⁰)]^2-(A) that was experimentally synthesized. Cavities of L¹ and L² macrocycles are found to match well with actinyl ions, but the one of L³ is a lot larger. Consequently, the L³ complexes have to adopt distorted geometry to energetically stabilize systems. Infrared vibrational spectra presented that the An=O stretching frequencies decrease in going from U, Np to Pu. This agrees with the trend of optimized bond lengths of An=O and bond orders. Topological analyses of quantum theory of atoms in molecule (QTAIM) indicate that the An-N bonds have largely ionic character. Depending on different actinyl source, free energies reacting with various macrocyclic ligands were calculated around 146.4 kJ·mol^-1, comparable to the calculated values of A. Time-dependent DFT calculations on four uranyl complexes well reproduced absorption spectra of experimentally reported analogue. The absorption bands in the near-IR and visible region have large contribution from ligand-to-metal charge transfer (LMCT), which is responsible for changes of solution color in the process of macrocyclic ligand sensing uranyl species.
- polypyrrollic uranyl/transuranyl complexes,
- QTAIM analysis,
- thermodynamic reaction,
- electronic spectroscopy,
- relativistic DFT
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