Journal
SEPARATION AND PURIFICATION TECHNOLOGY
Volume 282, Issue -, Pages -Publisher
ELSEVIER
DOI: 10.1016/j.seppur.2021.120046
Keywords
Solvent extraction; DAPhens; Uranyl separation; Steric hindrance; Single-crystal structure
Categories
Funding
- National Natural Science Foundation of China [21701073, 22076070]
- Gansu Province Science Foundation for Youths [20JR5RA224]
- Fundamental Research Funds for the Central Universities [lzujbky-2021-sp35]
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The asymmetric alkyl-substituted DAPhens showed higher affinity for UO22+ compared to symmetric analogues, likely due to decreased steric hindrance from methyl in the terminal groups. This was confirmed through the crystal and molecular structure of the solid-state complex, supporting their potential application as selective ligands.
Four asymmetric alkyl-substituted DAPhens (N,N'-Dimethyl-N,N'-Dialkyl-2,9-Diamide-1,10-Phenanthrolines) were synthesized and investigated as selective ligands for UO22+. The results confirm that the ligands have higher affinity for uranyl comparing to the symmetric analogues with the same 1,10-phenanthroline core moiety. The slope analysis indicated the formation of 1:1 (metal/ligand) extracting complex, which was identified in the organic phase as [UO2(DAPhen-4)(NO3)](+) complex ion by electrospray ionization mass spectrometry (ESI-MS). The superior affinity of the ligands for UO22+ over Th4+ and Eu3+ in solvent extraction was consistent with the stability constants of their complexes in acetonitrile obtained by UV-Vis spectroscopic titrations. The observed better affinity of the asymmetric alkyl-substituted DAPhens could originate from the less steric hindrance of methyl in the terminal groups, which was confirmed by the relatively mild distortion of the ligand structure in the uranyl complex according to the crystal and molecular structure of the solid-state complex [UO2(DAPhen-1) (NO3)](NO3)center dot(CH3OH) as characterized by single crystal X-ray diffraction.
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