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Article Abstract
The nitrilotriacetamide -octyl derivative ligand (NTAamide(-Oct)) is promising for minor actinide/lanthanide separation, yet periodic trends in its extraction and complexation across the lanthanide series remained unclear. This study systematically investigated its behavior with trivalent rare-earth ions (Ln, Y, and Sc) using solvent extraction, H NMR titration, UV-vis spectrophotometric titration, microcalorimetric titration, single-crystal X-ray diffractometry, ESI-MS, and FTIR. Key findings reveal opposing ionic radius dependencies. Solvent extraction showed that extraction efficiency negatively correlates with the ionic radius, decreasing with the ionic radius. Slope analysis indicated Sc forms 1:2 metal-ligand extracted complexes, while other RE ions form 1:1 complexes. Conversely, homogeneous and solid-state studies uniformly identified 1:2 stoichiometry for all RE complexes, with complexation strength positively dependent on the ionic radius, increasing as the ionic radius decreases. Overall, the extraction and complexation ability trends of NTAamide(-Oct) toward RE exhibit opposing tendencies. Combined with the results of solvent extraction and complexation studies, the compositions of the complexes formed by NTAamide(-Oct) with Sc or other RE are [ScL](NO) and [REL][RE(NO)] (L = NTAamide(-Oct)), respectively. Furthermore, an ion-pair extraction model is also proposed and discussed.
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| http://dx.doi.org/10.1021/acs.inorgchem.5c02125 | DOI Listing |
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