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.
journal_name
Nat Communjournal_title
Nature communicationsauthors
Ivanov AS,Leggett CJ,Parker BF,Zhang Z,Arnold J,Dai S,Abney CW,Bryantsev VS,Rao Ldoi
10.1038/s41467-017-01443-1subject
Has Abstractpub_date
2017-11-16 00:00:00pages
1560issue
1issn
2041-1723pii
10.1038/s41467-017-01443-1journal_volume
8pub_type
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