Highly Preorganized Ligand 1,10-Phenanthroline-2,9-dicarboxylic Acid for the Selective Recovery of Uranium from Seawater in the Presence of Competing Vanadium Species

Lashley, Mark A.; Ivanov, Alexander S.; Bryantsev, Vyacheslav S.; Dai, Sheng; Hancock, Robert D.

doi:10.1021/acs.inorgchem.6b02234

Title: Highly Preorganized Ligand 1,10-Phenanthroline-2,9-dicarboxylic Acid for the Selective Recovery of Uranium from Seawater in the Presence of Competing Vanadium Species

Journal Article · Fri Sep 30 00:00:00 EDT 2016 · Inorganic Chemistry

DOI:https://doi.org/10.1021/acs.inorgchem.6b02234· OSTI ID:1329747

Lashley, Mark A. ^[1]; Ivanov, Alexander S. ^[2]; Bryantsev, Vyacheslav S. ^[2]; Dai, Sheng ^[2]; Hancock, Robert D. ^[1]

Univ. of North Carolina Wilmington, NC (United States). Dept. of Chemistry and Biochemistry
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical Sciences Division

Studies of the complexation of new promising ligands with uranyl (UO₂²⁺) and other seawater cations can aid the development of more efficient, selective, and robust sorbents for the recovery of uranium from seawater. Here, we propose that the ligand design principles based on structural preorganization can be successfully applied to obtain a dramatic enhancement in UO₂²⁺ ion binding affinity and selectivity. This concept is exemplified through the investigation of the com-plexes of UO₂²⁺, VO²⁺, and VO²⁺ with the highly preorganized ligand PDA (1,10-phenanthroline-2,9-dicarboxylic acid) using a combination of fluores-cence and absorbance techniques, along with den-sity functional theory (DFT) calculations. Moreover, the measured stability constant value, log K1, of 16.5 for the UO₂²⁺/PDA complex is very high compared to uranyl complexes with other dicarboxylic ligands. Moreover, PDA exhibits strong selectivity for uranyl over vanadium ions, since the determined sta-bility constant values of the PDA complexes of the vanadium ions are quite low (V(IV) log K1 = 7.4, V(V) = 7.3). Finally, the structures of the corresponding UO₂²⁺, VO²⁺, and VO²⁺ complexes with PDA were identified by systematic DFT calculations, and helped to interpret the stronger binding affinity for uranium over the vanadium ions. Due to its high chemical stability, selectivity, and structural preor-ganization for UO₂²⁺ complexation, PDA is a very promising candidate that can be potentially used in the development of novel adsorbent materials for the selective extraction of uranium from sea-water.

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Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Nuclear Energy (NE)

Grant/Contract Number:: AC05-00OR22725; AC02-05CH11231

OSTI ID:: 1329747

Journal Information:: Inorganic Chemistry, Vol. 55, Issue 20; ISSN 0020-1669

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 39 works

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