The Influence of Linker Geometry in Bis(3-hydroxy-N-methyl-pyridin-2-one) Ligands on Solution Phase Uranyl Affinity

被引：24
作者：
Szigethy, Geza [1 ,2 ]
Raymond, Kenneth N. [1 ,2 ]
机构：
[1] Univ Calif Berkeley, Lawrence Berkeley Lab, Div Chem Sci, Berkeley, CA 94720 USA
[2] Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA
来源：
CHEMISTRY-A EUROPEAN JOURNAL | 2011年 / 17卷 / 06期
关键词：
analytical methods; ligand effects; speciation; thermodynamics; uranium; STEREOGNOSTIC COORDINATION CHEMISTRY; SEQUESTERING AGENTS; CHELATING-AGENTS; EQUILIBRIUM-CONSTANTS; CRYSTAL-STRUCTURE; UO22+ COMPLEXES; DESIGN; URANIUM(VI); ACTINIDES; PROGRAM;
D O I：
10.1002/chem.201002372
中图分类号：
O6 [化学];
学科分类号：
0703 ;
摘要：
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.
引用
收藏
页码：1818 / 1827
页数：10
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