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 · Mon Aug 01 00:00:00 EDT 2016 · Physical Chemistry Chemical Physics. PCCP

DOI:https://doi.org/10.1039/C6CP04772F· OSTI ID:1295145

Abney, C. W. ^[1]; Das, S. ^[1]; Mayes, R. T. ^[1]; Kuo, L. -J. ^[2]; Wood, J. ^[2]; Gill, G. ^[2]; Piechowicz, M. ^[3]; Lin, Z. ^[3]; Lin, W. ^[3]; Dai, S. ^[1]

Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Univ. of Chicago, Chicago, IL (United States)

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 platform for achieving this separation, yet 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 a polymer. Samples exposed to seawater also display a feature consistent with a 2-oxo-bridged transition metal, suggesting formation of an in situ specific binding site. As a result, these findings challenge long held assumptions and provide new opportunities for the design of advanced adsorbent materials.

View Accepted Manuscript (DOE)

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

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

Grant/Contract Number:: AC02-06CH11357; AC05-00OR22725

OSTI ID:: 1295145

Alternate ID(s):: OSTI ID: 1329436
OSTI ID: 1340747

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

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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