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

Ivanov, Alexander S.; Leggett, Christina J.; Parker, Bernard F.; Zhang, Zhicheng; Arnold, John; Dai, Sheng; Abney, Carter W.; Bryantsev, Vyacheslav S.; Rao, Linfeng

doi:10.1038/s41467-017-01443-1

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

Journal Article · Thu Nov 16 00:00:00 EST 2017 · Nature Communications

DOI:https://doi.org/10.1038/s41467-017-01443-1· OSTI ID:1419451

^[1]; Leggett, Christina J. ^[2]; ^[3]; Zhang, Zhicheng ^[4]; Arnold, John ^[3]; ^[1]; Abney, Carter W. ^[1]; ^[1]; Rao, Linfeng ^[4]

Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); US Nuclear Regulatory Commission, Rockville, MD (United States)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Univ. of California, Berkeley, CA (United States)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)

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. Here in this paper, 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.

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: AC02-05CH11231; AC02-06CH11357; AC02-76SF00515; AC05-00OR22725

OSTI ID:: 1419451

Alternate ID(s):: OSTI ID: 1423083

Journal Information:: Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 8; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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