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Title: Uranium recovery from seawater: development of fiber adsorbents prepared via atom-transfer radical polymerization

Abstract

We developed a novel adsorbent preparation method using atom-transfer radical polymerization (ATRP) combined with radiation-induced graft polymerization (RIGP) in order to synthesize an adsorbent for uranium recovery from seawater. Furthermore, the ATRP method allowed a much higher degree of grafting on the adsorbent fibers (595 2818%) than that allowed by RIGP alone. The adsorbents were prepared with varied composition of amidoxime groups and hydrophilic acrylate groups. The successful preparation revealed that both ligand density and hydrophilicity were critical for optimal performance of the adsorbents. Adsorbents synthesized in this study showed a relatively high performance (141 179 mg/g at 49 62 % adsorption) in laboratory screening tests using a uranium concentration of ~6 ppm. This performance is much higher than that of known commercial adsorbents. However, actual seawater experiment showed impeded performance compared to the recently reported high-surface-area-fiber adsorbents, due to slow adsorption kinetics. The impeded performance motivated an investigation of the effect of hydrophilic block addition on the graft chain terminus. The addition of hydrophilic block on the graft chain terminus nearly doubled the uranium adsorption capacity in seawater, from 1.56 mg/g to 3.02 mg/g. Our investigation revealed the importance of polymer chain conformation, in addition to ligand and hydrophilicmore » group ratio, for advanced adsorbent synthesis for uranium recovery from seawater.« less

Authors:
 [1];  [2];  [1];  [3];  [3];  [1];  [4];  [4];  [1];  [5];  [6]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical Sciences Division
  2. Univ. of Tennessee, Knoxville, TN (United States). Dept. of Chemistry
  3. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Energy and Transportation Science Division
  4. Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Marine Science Lab.
  5. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science and Technology Division
  6. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical Sciences Division; Univ. of Tennessee, Knoxville, TN (United States). Marine Sciences Lab.
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1149751
DOE Contract Number:
AC05-00OR22725
Resource Type:
Journal Article
Resource Relation:
Journal Name: Journal of Materials Chemistry. A; Journal Volume: 2; Journal Issue: 35
Country of Publication:
United States
Language:
English
Subject:
07 ISOTOPE AND RADIATION SOURCES; uranium recovery; seawater; polymer fiber; adsorbent; atom-transfer radical polymerization

Citation Formats

Saito, Tomonori, Brown, Suree, Chatterjee, Sabornie, Kim, Jungseung, Tsouris, Costas, Mayes, Richard T., Kuo, Li-Jung, Gill, Gary, Oyola, Yatsandra, Janke, Christopher J., and Dai, Sheng. Uranium recovery from seawater: development of fiber adsorbents prepared via atom-transfer radical polymerization. United States: N. p., 2014. Web. doi:10.1039/C4TA03276D.
Saito, Tomonori, Brown, Suree, Chatterjee, Sabornie, Kim, Jungseung, Tsouris, Costas, Mayes, Richard T., Kuo, Li-Jung, Gill, Gary, Oyola, Yatsandra, Janke, Christopher J., & Dai, Sheng. Uranium recovery from seawater: development of fiber adsorbents prepared via atom-transfer radical polymerization. United States. doi:10.1039/C4TA03276D.
Saito, Tomonori, Brown, Suree, Chatterjee, Sabornie, Kim, Jungseung, Tsouris, Costas, Mayes, Richard T., Kuo, Li-Jung, Gill, Gary, Oyola, Yatsandra, Janke, Christopher J., and Dai, Sheng. Mon . "Uranium recovery from seawater: development of fiber adsorbents prepared via atom-transfer radical polymerization". United States. doi:10.1039/C4TA03276D.
@article{osti_1149751,
title = {Uranium recovery from seawater: development of fiber adsorbents prepared via atom-transfer radical polymerization},
author = {Saito, Tomonori and Brown, Suree and Chatterjee, Sabornie and Kim, Jungseung and Tsouris, Costas and Mayes, Richard T. and Kuo, Li-Jung and Gill, Gary and Oyola, Yatsandra and Janke, Christopher J. and Dai, Sheng},
abstractNote = {We developed a novel adsorbent preparation method using atom-transfer radical polymerization (ATRP) combined with radiation-induced graft polymerization (RIGP) in order to synthesize an adsorbent for uranium recovery from seawater. Furthermore, the ATRP method allowed a much higher degree of grafting on the adsorbent fibers (595 2818%) than that allowed by RIGP alone. The adsorbents were prepared with varied composition of amidoxime groups and hydrophilic acrylate groups. The successful preparation revealed that both ligand density and hydrophilicity were critical for optimal performance of the adsorbents. Adsorbents synthesized in this study showed a relatively high performance (141 179 mg/g at 49 62 % adsorption) in laboratory screening tests using a uranium concentration of ~6 ppm. This performance is much higher than that of known commercial adsorbents. However, actual seawater experiment showed impeded performance compared to the recently reported high-surface-area-fiber adsorbents, due to slow adsorption kinetics. The impeded performance motivated an investigation of the effect of hydrophilic block addition on the graft chain terminus. The addition of hydrophilic block on the graft chain terminus nearly doubled the uranium adsorption capacity in seawater, from 1.56 mg/g to 3.02 mg/g. Our investigation revealed the importance of polymer chain conformation, in addition to ligand and hydrophilic group ratio, for advanced adsorbent synthesis for uranium recovery from seawater.},
doi = {10.1039/C4TA03276D},
journal = {Journal of Materials Chemistry. A},
number = 35,
volume = 2,
place = {United States},
year = {Mon Aug 04 00:00:00 EDT 2014},
month = {Mon Aug 04 00:00:00 EDT 2014}
}