A report on emergent uranyl binding phenomena by an amidoxime phosphonic acid co-polymer
Abstract
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.
- Authors:
-
- 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)
- Publication Date:
- Research Org.:
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- Sponsoring Org.:
- USDOE Office of Nuclear Energy (NE), Fuel Cycle Technologies (NE-5)
- OSTI Identifier:
- 1295145
- Grant/Contract Number:
- AC05-00OR22725; AC02-06CH11357
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Physical Chemistry Chemical Physics. PCCP
- Additional Journal Information:
- Journal Name: Physical Chemistry Chemical Physics. PCCP; Journal ID: ISSN 1463-9076
- Publisher:
- Royal Society of Chemistry
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS; 36 MATERIALS SCIENCE; XAFS; uranium; seawater; emergent phenomena; polymer
Citation Formats
Abney, C. W., Das, S., Mayes, R. T., Kuo, L. -J., Wood, J., Gill, G., Piechowicz, M., Lin, Z., Lin, W., and Dai, S. A report on emergent uranyl binding phenomena by an amidoxime phosphonic acid co-polymer. United States: N. p., 2016.
Web. doi:10.1039/C6CP04772F.
Abney, C. W., Das, S., Mayes, R. T., Kuo, L. -J., Wood, J., Gill, G., Piechowicz, M., Lin, Z., Lin, W., & Dai, S. A report on emergent uranyl binding phenomena by an amidoxime phosphonic acid co-polymer. United States. https://doi.org/10.1039/C6CP04772F
Abney, C. W., Das, S., Mayes, R. T., Kuo, L. -J., Wood, J., Gill, G., Piechowicz, M., Lin, Z., Lin, W., and Dai, S. Mon .
"A report on emergent uranyl binding phenomena by an amidoxime phosphonic acid co-polymer". United States. https://doi.org/10.1039/C6CP04772F. https://www.osti.gov/servlets/purl/1295145.
@article{osti_1295145,
title = {A report on emergent uranyl binding phenomena by an amidoxime phosphonic acid co-polymer},
author = {Abney, C. W. and Das, S. and Mayes, R. T. and Kuo, L. -J. and Wood, J. and Gill, G. and Piechowicz, M. and Lin, Z. and Lin, W. and Dai, S.},
abstractNote = {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.},
doi = {10.1039/C6CP04772F},
journal = {Physical Chemistry Chemical Physics. PCCP},
number = ,
volume = ,
place = {United States},
year = {Mon Aug 01 00:00:00 EDT 2016},
month = {Mon Aug 01 00:00:00 EDT 2016}
}
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