Origin of the unusually strong and selective binding of vanadium by polyamidoximes in seawater

Alexander S. Ivanov, Christina J. Leggett, Bernard F. Parker, Zhicheng Zhang, John Arnold, Sheng Dai, Carter W. Abney (), Vyacheslav S. Bryantsev () and Linfeng Rao ()
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Alexander S. Ivanov: Oak Ridge National Laboratory
Christina J. Leggett: Lawrence Berkeley National Laboratory
Bernard F. Parker: Lawrence Berkeley National Laboratory
Zhicheng Zhang: Lawrence Berkeley National Laboratory
John Arnold: Lawrence Berkeley National Laboratory
Sheng Dai: Oak Ridge National Laboratory
Carter W. Abney: Oak Ridge National Laboratory
Vyacheslav S. Bryantsev: Oak Ridge National Laboratory
Linfeng Rao: Lawrence Berkeley National Laboratory

Nature Communications, 2017, vol. 8, issue 1, 1-10

Abstract: Abstract Amidoxime-functionalized polymeric adsorbents are the current state-of-the-art materials for collecting uranium (U) from seawater. However, marine tests show that vanadium (V) is preferentially extracted over U and many other cations. Herein, we report a complementary and comprehensive investigation integrating ab initio simulations with thermochemical titrations and XAFS spectroscopy to understand the unusually strong and selective binding of V by polyamidoximes. While the open-chain amidoxime functionalities do not bind V, the cyclic imide-dioxime group of the adsorbent forms a peculiar non-oxido V5+ complex, exhibiting the highest stability constant value ever observed for the V5+ species. XAFS analysis of adsorbents following deployment in environmental seawater confirms V binding solely by the imide-dioximes. Our fundamental findings offer not only guidance for future optimization of selectivity in amidoxime-based sorbent materials, but may also afford insight to understanding the extensive accumulation of V in some marine organisms.

Date: 2017
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DOI: 10.1038/s41467-017-01443-1

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