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Title: Successful Coupling of a Bis-Amidoxime Uranophile with a Hydrophilic Backbone for Selective Uranium Sequestration

Abstract

The amidoxime group (-RNH2NOH) has long been used to extract uranium from seawater on account of its high affinity toward uranium. The development of tunable sorbent materials for uranium sequestration remains a research priority as well as a significant challenge. Herein, we report the design, synthesis, and uranium sorption properties of bis-amidoxime-functionalized polymeric materials (BAP 1–3). Bifunctional amidoxime monomers were copolymerized with an acrylamide cross-linker to obtain bis-amidoxime incorporation as high as 2 mmol g–1 after five synthetic steps. The resulting sorbents were able to uptake nearly 600 mg of uranium per gram of polymer after 37 days of contact with a seawater simulant containing 8 ppm uranium. Moreover, the polymeric materials exhibited low vanadium uptake with a maximum capacity of 128 mg of vanadium per gram of polymer. This computationally predicted and experimentally realized selectivity of uranium over vanadium, nearly 5 to 1 w/w, is one of the highest reported to date and represents an advancement in the rational design of sorbent materials with high uptake capacity and selectivity.

Authors:
 [1]; ORCiD logo [2];  [1];  [1];  [3];  [1]; ORCiD logo [4]; ORCiD logo [1]
  1. Department of Chemistry, University of Chicago, 929 E. 57th Street, Chicago, Illinois 60637, United States
  2. Oak Ridge National Laboratory, P.O. Box 2008, MS-6201, Oak Ridge, Tennessee 37831-6181, United States
  3. Department of Chemistry, University of Chicago, 929 E. 57th Street, Chicago, Illinois 60637, United States; Shanghai Key Laboratory of Advanced Polymeric Materials, School of Materials Science and Engineering, East China University of Science and Technology, Shanghai 200237, China
  4. Shanghai Key Laboratory of Advanced Polymeric Materials, School of Materials Science and Engineering, East China University of Science and Technology, Shanghai 200237, China
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
Sponsoring Org.:
USDOE Office of Nuclear Energy (NE)
OSTI Identifier:
1379433
Resource Type:
Journal Article
Journal Name:
ACS Applied Materials and Interfaces
Additional Journal Information:
Journal Volume: 9; Journal Issue: 33; Journal ID: ISSN 1944-8244
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
ENGLISH
Subject:
36 MATERIALS SCIENCE; amidoxime; cooperative binding; DFT; seawater; uranium extraction

Citation Formats

Piechowicz, Marek, Abney, Carter W., Thacker, Nathan C., Gilhula, James C., Wang, Youfu, Veroneau, Samuel S., Hu, Aiguo, and Lin, Wenbin. Successful Coupling of a Bis-Amidoxime Uranophile with a Hydrophilic Backbone for Selective Uranium Sequestration. United States: N. p., 2017. Web. doi:10.1021/acsami.7b04656.
Piechowicz, Marek, Abney, Carter W., Thacker, Nathan C., Gilhula, James C., Wang, Youfu, Veroneau, Samuel S., Hu, Aiguo, & Lin, Wenbin. Successful Coupling of a Bis-Amidoxime Uranophile with a Hydrophilic Backbone for Selective Uranium Sequestration. United States. doi:10.1021/acsami.7b04656.
Piechowicz, Marek, Abney, Carter W., Thacker, Nathan C., Gilhula, James C., Wang, Youfu, Veroneau, Samuel S., Hu, Aiguo, and Lin, Wenbin. Thu . "Successful Coupling of a Bis-Amidoxime Uranophile with a Hydrophilic Backbone for Selective Uranium Sequestration". United States. doi:10.1021/acsami.7b04656.
@article{osti_1379433,
title = {Successful Coupling of a Bis-Amidoxime Uranophile with a Hydrophilic Backbone for Selective Uranium Sequestration},
author = {Piechowicz, Marek and Abney, Carter W. and Thacker, Nathan C. and Gilhula, James C. and Wang, Youfu and Veroneau, Samuel S. and Hu, Aiguo and Lin, Wenbin},
abstractNote = {The amidoxime group (-RNH2NOH) has long been used to extract uranium from seawater on account of its high affinity toward uranium. The development of tunable sorbent materials for uranium sequestration remains a research priority as well as a significant challenge. Herein, we report the design, synthesis, and uranium sorption properties of bis-amidoxime-functionalized polymeric materials (BAP 1–3). Bifunctional amidoxime monomers were copolymerized with an acrylamide cross-linker to obtain bis-amidoxime incorporation as high as 2 mmol g–1 after five synthetic steps. The resulting sorbents were able to uptake nearly 600 mg of uranium per gram of polymer after 37 days of contact with a seawater simulant containing 8 ppm uranium. Moreover, the polymeric materials exhibited low vanadium uptake with a maximum capacity of 128 mg of vanadium per gram of polymer. This computationally predicted and experimentally realized selectivity of uranium over vanadium, nearly 5 to 1 w/w, is one of the highest reported to date and represents an advancement in the rational design of sorbent materials with high uptake capacity and selectivity.},
doi = {10.1021/acsami.7b04656},
journal = {ACS Applied Materials and Interfaces},
issn = {1944-8244},
number = 33,
volume = 9,
place = {United States},
year = {2017},
month = {8}
}