Effect of Counteranions on the Extraction and Complexation of Trivalent Lanthanides with Tetradentate Phenanthroline-Derived Phosphonate Ligands

Inorganic Chemistry
Xiao YangCheng-Liang Xiao

Abstract

Soft-hard-donor-combined ligands are a type of promising extractant for actinide and lanthanide separation. In this work, the effects of counteranions (Cl-, NO3-, and ClO4-) on the extraction and complexation behaviors of a recently reported tetradentate phenanthroline-derived phosphonate (POPhen) ligand toward lanthanides were thoroughly investigated using solvent extraction, NMR titration, UV-vis titration, and single-crystal X-ray diffraction measurements. It is found that C4-POPhen showed excellent extraction and selectivity toward heavy lanthanides [Lu(III)] compared to light lanthanides, particularly with the counterion of ClO4- and at low acidity. NMR titration studies demonstrated that both 1:1 and 1:2 Lu(III)/C4-POPhen complexes were formed in a CD3OD solution with all three counteranions and the 1:2 species was easier to form in a complexation of C4-POPhen with Lu(ClO4)3 under the same conditions. Furthermore, the stability constants of Nd(III) complexation with C4-POPhen in the counteranions of Cl-, NO3-, and ClO4- systems were determined through UV-vis titration, and a much larger value of log β of complexes was found in the ClO4- system, which was in good agreement with the results of solvent extraction. In additio...Continue Reading

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