NDLI: XAFS investigation of polyamidoxime-bound uranyl contests the paradigm from small molecule studies

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XAFS investigation of polyamidoxime-bound uranyl contests the paradigm from small molecule studies

Content Provider	United States Department of Energy Office of Scientific and Technical Information (OSTI.GOV)
Author	Mayes, Richard T. Piechowicz, Marek Veith, Gabriel M. Abney, C. W. Bryantsev, V. S.
Organization	Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Abstract	In this study, limited resource availability and population growth have motivated interest in harvesting valuable metals from unconventional reserves, but developing selective adsorbents for this task requires structural knowledge of metal binding environments. Amidoxime polymers have been identified as the most promising platform for large-scale extraction of uranium from seawater. However, despite more than 30 years of research, the uranyl coordination environment on these adsorbents has not been positively identified. We report the first XAFS investigation of polyamidoxime-bound uranyl, with EXAFS fits suggesting a cooperative chelating model, rather than the tridentate or η² motifs proposed by small molecule and computational studies. Samples exposed to environmental seawater also display a feature consistent with a μ²-oxo-bridged transition metal in the uranyl coordination sphere, suggesting in situ formation of a specific binding site or mineralization of uranium on the polymer surface. These unexpected findings challenge several long-held assumptions and have significant implications for development of polymer adsorbents with high selectivity.
Sponsorship	USDOE Office of Nuclear Energy (NE)
Related Links	https://www.osti.gov/biblio/1244198
Starting Page	448
Ending Page	453
Page Count	6
File Format	PDF
ISSN	17545692
DOI	10.1039/C5EE02913A
Journal	Energy & Environmental Science
Volume Number	9
Issue Number	2
Language	English
Publisher	Royal Society of Chemistry
Publisher Date	2015-11-12
Publisher Place	United States
Access Restriction	Open
Subject Keyword	INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY XAFS uranium nuclear fuel cycle amidoxime seawater unconventional resources
Content Type	Text
Resource Type	Article
Subject	Environmental Chemistry Pollution Renewable Energy, Sustainability and the Environment Nuclear Energy and Engineering

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