Journal
CHEMISTRY-A EUROPEAN JOURNAL
Volume 17, Issue 6, Pages 1818-1827Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/chem.201002372
Keywords
analytical methods; ligand effects; speciation; thermodynamics; uranium
Categories
Funding
- Office of Science, Office of Basic Energy Sciences
- Division of Chemical Sciences, Geosciences, and Biosciences of the U.S. Department of Energy at LBNL [DE-AC02-05CH11231]
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Seven water-soluble, tetradentate bis(3-hydroxy-N-methyl-pyridin-2-one) (bis-Me-3,2-HOPO) ligands were synthesized that vary only in linker geometry and rigidity. Solution-phase thermodynamic measurements were conducted between pH 1.6 and pH 9.0 to determine the effects of these variations on proton and uranyl cation affinity. Proton affinity decreases by introduction of the solubilizing triethylene glycol group as compared to unsubstituted reference ligands. Uranyl affinity was found to follow no discernable trends with incremental geometric modification. The butyl-linked 4li-Me-3,2-HOPO ligand exhibited the highest uranyl affinity, consistent with prior in vivo decorporation results. Of the rigidly-linked ligands, the o-phenylene linker imparted the best uranyl affinity to the bis-Me-3,2-HOPO ligand platform.
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