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

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 η 2 motifs proposed by small molecule and computational studies. Samples exposed to environmental seawater also display a feature consistent with a μ 2-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.

Authors:
 [1];  [2];  [2];  [1];  [1];  [2];  [3];  [1]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  2. Univ. of Chicago, Chicago, IL (United States)
  3. Univ. of Chicago, Chicago, IL (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Nuclear Energy (NE)
OSTI Identifier:
1244198
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Energy & Environmental Science
Additional Journal Information:
Journal Volume: 9; Journal Issue: 2; Journal ID: ISSN 1754-5692
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; XAFS; uranium; nuclear fuel cycle; amidoxime; seawater; unconventional resources

Citation Formats

Mayes, Richard T., Piechowicz, Marek, Lin, Zekai, Veith, Gabriel M., Dai, Sheng, Lin, Wenbin, Abney, C. W., and Bryantsev, V. S. XAFS investigation of polyamidoxime-bound uranyl contests the paradigm from small molecule studies. United States: N. p., 2015. Web. doi:10.1039/C5EE02913A.
Mayes, Richard T., Piechowicz, Marek, Lin, Zekai, Veith, Gabriel M., Dai, Sheng, Lin, Wenbin, Abney, C. W., & Bryantsev, V. S. XAFS investigation of polyamidoxime-bound uranyl contests the paradigm from small molecule studies. United States. doi:10.1039/C5EE02913A.
Mayes, Richard T., Piechowicz, Marek, Lin, Zekai, Veith, Gabriel M., Dai, Sheng, Lin, Wenbin, Abney, C. W., and Bryantsev, V. S. Thu . "XAFS investigation of polyamidoxime-bound uranyl contests the paradigm from small molecule studies". United States. doi:10.1039/C5EE02913A. https://www.osti.gov/servlets/purl/1244198.
@article{osti_1244198,
title = {XAFS investigation of polyamidoxime-bound uranyl contests the paradigm from small molecule studies},
author = {Mayes, Richard T. and Piechowicz, Marek and Lin, Zekai and Veith, Gabriel M. and Dai, Sheng and Lin, Wenbin and Abney, C. W. and Bryantsev, V. S.},
abstractNote = {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.},
doi = {10.1039/C5EE02913A},
journal = {Energy & Environmental Science},
number = 2,
volume = 9,
place = {United States},
year = {2015},
month = {11}
}

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Cited by: 22 works
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    • Kobuke, Yoshiaki; Tanaka, Hiromitsu; Ogoshi, Hisanobu
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    • Dalton Transactions, Vol. 42, Issue 16
    • DOI: 10.1039/c3dt32940b

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    • Den Auwer, Christophe; Simoni, Eric; Conradson, Steven
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    Uranium Incorporation into Amorphous Silica
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    • Massey, Michael S.; Lezama-Pacheco, Juan S.; Nelson, Joey M.
    • Environmental Science & Technology, Vol. 48, Issue 15
    • DOI: 10.1021/es501064m

    The adsorption mechanism of uranium(VI) from seawater on a macroporous fibrous polymeric adsorbent containing amidoxime chelating functional group
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    Uptake of Uranium from Seawater by Amidoxime-Based Polymeric Adsorbent: Field Experiments, Modeling, and Updated Economic Assessment
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    • Kim, Jungseung; Tsouris, Costas; Oyola, Yatsandra
    • Industrial & Engineering Chemistry Research, Vol. 53, Issue 14
    • DOI: 10.1021/ie4039828

    Review of cost estimates for uranium recovery from seawater
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    Coordination chemistry in the ocean
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    Sequestering uranium from seawater: binding strength and modes of uranyl complexes with glutarimidedioxime
    journal, January 2012

    • Tian, Guoxin; Teat, Simon J.; Zhang, Zhiyong
    • Dalton Transactions, Vol. 41, Issue 38
    • DOI: 10.1039/c2dt30978e

    A new series of pillared uranyl-vanadates based on uranophane-type sheets in the uranium-vanadium-linear alkyl diamine systems
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    • Jouffret, Laurent; Rivenet, Murielle; Abraham, Francis
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    • DOI: 10.1016/j.jssc.2009.10.020

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    • Geochimica et Cosmochimica Acta, Vol. 73, Issue 20
    • DOI: 10.1016/j.gca.2009.07.002

    Recovery of Uranium from Seawater: A Review of Current Status and Future Research Needs
    journal, January 2013


    Molecular simulation of the diffusion of uranyl carbonate species in aqueous solution
    journal, September 2010


    Highly porous and stable metal–organic frameworks for uranium extraction
    journal, January 2013

    • Carboni, Michaël; Abney, Carter W.; Liu, Shubin
    • Chemical Science, Vol. 4, Issue 6, p. 2396-2402
    • DOI: 10.1039/c3sc50230a

    Raw material criticality in the context of classical risk assessment
    journal, June 2015


    Seawater Uranium Sorbents: Preparation from a Mesoporous Copolymer Initiator by Atom-Transfer Radical Polymerization
    journal, October 2013

    • Yue, Yanfeng; Mayes, Richard T.; Kim, Jungseung
    • Angewandte Chemie International Edition, Vol. 52, Issue 50
    • DOI: 10.1002/anie.201307825

    Speciation of Uranium in Sediments before and after In situ Biostimulation
    journal, March 2008

    • Kelly, Shelly D.; Kemner, Kenneth M.; Carley, Jack
    • Environmental Science & Technology, Vol. 42, Issue 5
    • DOI: 10.1021/es071764i

    Sorption of Uranium(VI) onto Lanthanum Phosphate Surfaces
    journal, October 2002

    • Ordoñez-Regil, E.; Drot, R.; Simoni, E.
    • Langmuir, Vol. 18, Issue 21
    • DOI: 10.1021/la025674x

    A protein engineered to bind uranyl selectively and with femtomolar affinity
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    • Zhou, Lu; Bosscher, Mike; Zhang, Changsheng
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    • DOI: 10.1038/nchem.1856

    Spectroscopic Confirmation of Uranium(VI)−Carbonato Adsorption Complexes on Hematite
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    • Bargar, John R.; Reitmeyer, Rebecca; Davis, James A.
    • Environmental Science & Technology, Vol. 33, Issue 14
    • DOI: 10.1021/es990048g

    Highly selective extraction of the uranyl ion with hydrophobic amidoxime-functionalized ionic liquids via η2 coordination
    journal, January 2012

    • Barber, Patrick S.; Kelley, Steven P.; Rogers, Robin D.
    • RSC Advances, Vol. 2, Issue 22
    • DOI: 10.1039/c2ra21344c

    Life-cycle impacts from novel thorium–uranium-fuelled nuclear energy systems
    journal, September 2015


    Uranium Uptake from Aqueous Solution by Interaction with Goethite, Lepidocrocite, Muscovite, and Mackinawite:  An X-ray Absorption Spectroscopy Study
    journal, March 2000

    • Moyes, Lesley N.; Parkman, Richard H.; Charnock, John M.
    • Environmental Science & Technology, Vol. 34, Issue 6
    • DOI: 10.1021/es990703k

    Structure of di-.mu.-aquo-bis(dioxobis(nitrato)uranium(VI)) diimidazole, [UO2 (NO3)2(H2O)].2C3H4N2, a water bridged dimer of uranyl nitrate
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