A report on emergent uranyl binding phenomena by an amidoxime phosphonic acid co-polymer

Abney, C. W.; Das, S.; Mayes, R. T.; Kuo, L. -J.; Wood, J.; Gill, G.; Piechowicz, M.; Lin, Z.; Lin, W.; Dai, S.

doi:10.1039/c6cp04772f

A report on emergent uranyl binding phenomena by an amidoxime phosphonic acid co-polymer

Journal Article · Fri Jan 01 04:00:00 EST 2016 · Physical Chemistry Chemical Physics. PCCP

DOI:https://doi.org/10.1039/c6cp04772f· OSTI ID:1340747

Abney, C. W.; Das, S.; Mayes, R. T.; Kuo, L. -J.; Wood, J.; Gill, G.; Piechowicz, M.; Lin, Z.; Lin, W.; Dai, S.

The development of technology to harvest the uranium dissolved in seawater would enable access to vast quantities of this critical metal for nuclear power generation. Amidoxime polymers are the most promising platforms for achieving this separation, yet the design of advanced adsorbents is hindered by uncertainty regarding the uranium binding mode. In this work we use XAFS to investigate the uranium coordination environment in an amidoxime–phosphonic acid copolymer adsorbent. In contrast to the binding mode predicted computationally and from small molecule studies, a cooperative chelating model is favoured, attributable to emergent behavior resulting from inclusion of amidoxime in the polymer. Samples exposed to seawater also display a feature consistent with a μ2-oxo-bridged transition metal, suggesting the formation of an in situ specific binding site. These findings challenge long held assumptions and provide new opportunities for the design of advanced adsorbent materials.

Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (US)

Sponsoring Organization:: USDOE Office of Nuclear Energy (NE), Fuel Cycle Technologies (NE-5)

DOE Contract Number:: AC05-76RL01830

OSTI ID:: 1340747

Report Number(s):: PNNL-SA-120240; AF5855000

Journal Information:: Physical Chemistry Chemical Physics. PCCP, Journal Name: Physical Chemistry Chemical Physics. PCCP Journal Issue: 34 Vol. 18; ISSN 1463-9076; ISSN PPCPFQ

Publisher:: Royal Society of Chemistry

Country of Publication:: United States

Language:: English

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