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Title: Uranium Recovery from Seawater: Development of Fiber Adsorbents Prepared via Atom-Transfer Radical Polymerization

Abstract

Uranium exists uniformly at a concentration of ~3.3 ppb in seawater. The extraction of uranium from seawater presents a very attractive alternative source of uranium for nuclear fuel needs.

Authors:
; ; ; ; ; ; ; ; ; ;
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1171889
Report Number(s):
PNNL-SA-104178
AF5855000
DOE Contract Number:
AC05-76RL01830
Resource Type:
Journal Article
Resource Relation:
Journal Name: Journal of Materials Chemistry A, 2(35):14674-14681
Country of Publication:
United States
Language:
English

Citation Formats

Saito, Tomonori, Brown, Suree, Chatterjee, Sabornie, Kim, Jungseung, Tsouris, Constantinos, Mayes, Richard, Kuo, Li-Jung, Gill, Gary A., Oyola, Yatsandra, Janke, C., 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, Constantinos, Mayes, Richard, Kuo, Li-Jung, Gill, Gary A., Oyola, Yatsandra, Janke, C., & 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, Constantinos, Mayes, Richard, Kuo, Li-Jung, Gill, Gary A., Oyola, Yatsandra, Janke, C., and Dai, Sheng. Wed . "Uranium Recovery from Seawater: Development of Fiber Adsorbents Prepared via Atom-Transfer Radical Polymerization". United States. doi:10.1039/C4TA03276D.
@article{osti_1171889,
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, Constantinos and Mayes, Richard and Kuo, Li-Jung and Gill, Gary A. and Oyola, Yatsandra and Janke, C. and Dai, Sheng},
abstractNote = {Uranium exists uniformly at a concentration of ~3.3 ppb in seawater. The extraction of uranium from seawater presents a very attractive alternative source of uranium for nuclear fuel needs.},
doi = {10.1039/C4TA03276D},
journal = {Journal of Materials Chemistry A, 2(35):14674-14681},
number = ,
volume = ,
place = {United States},
year = {Wed Jul 09 00:00:00 EDT 2014},
month = {Wed Jul 09 00:00:00 EDT 2014}
}
  • 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 62more » % 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.« less
  • The need to secure future supplies of energy attracts researchers in several countries to a vast resource of nuclear energy fuel: uranium in seawater (estimated at 4.5 billion tons in seawater). In this study, we developed effective adsorbent fibers for the recovery of uranium from seawater via atom-transfer radical polymerization (ATRP) from a poly- (vinyl chloride)-co-chlorinated poly(vinyl chloride) (PVC-co-CPVC) fiber. ATRP was employed in the surface graft polymerization of acrylonitrile (AN) and tert-butyl acrylate (tBA), precursors for uranium-interacting functional groups, from PVC-co-CPVC fiber. The [tBA]/[AN] was systematically varied to identify the optimal ratio between hydrophilic groups (from tBA) and uranyl-bindingmore » ligands (from AN). The best performing adsorbent fiber, the one with the optimal [tBA]/[AN] ratio and a high degree of grafting (1390%), demonstrated uranium adsorption capacities that are significantly greater than those of the Japan Atomic Energy Agency (JAEA) reference fiber in natural seawater tests (2.42-3.24 g/kg in 42 days of seawater exposure and 5.22 g/kg in 49 days of seawater exposure, versus 1.66 g/kg in 42 days of seawater exposure and 1.71 g/kg in 49 days of seawater exposure for JAEA). Adsorption of other metal ions from seawater and their corresponding kinetics were also studied. The grafting of alternative monomers for the recovery of uranium from seawater is now under development by this versatile technique of ATRP.« less
  • The need to secure future supplies of energy attracts researchers in several countries to a vast resource of nuclear energy fuel: uranium in seawater (estimated at 4.5 billion tons in seawater). In this study, we developed effective adsorbent fibers for the recovery of uranium from seawater via atom-transfer radical polymerization (ATRP) from a poly-(vinyl chloride)-co-chlorinated poly(vinyl chloride) (PVC-co-CPVC) fiber. ATRP was employed in the surface graft polymerization of acrylonitrile (AN) and tert-butyl acrylate (tBA), precursors for uranium-interacting functional groups, from PVC-co-CPVC fiber. The [tBA]/[AN] was systematically varied to identify the optimal ratio between hydrophilic groups (from tBA) and uranyl-binding ligandsmore » (from AN). The best performing adsorbent fiber, the one with the optimal [tBA]/[AN] ratio and a high degree of grafting (1390%), demonstrated uranium adsorption capacities that are significantly greater than those of the Japan Atomic Energy Agency (JAEA) reference fiber in natural seawater tests (2.42 3.24 g/kg in 42 days of seawater exposure and 5.22 g/kg in 49 days of seawater exposure, versus 1.66 g/kg in 42 days of seawater exposure and 1.71 g/kg in 49 days of seawater exposure for JAEA). Lastly, adsorption of other metal ions from seawater and their corresponding kinetics were also studied. The grafting of alternative monomers for the recovery of uranium from seawater is now under development by this versatile technique of ATRP.« less
  • Brush-on-brush structures are proposed as one method to overcome support effects in grafted polymers. Utilizing glycidyl methacrylate (GMA) grafted on polyethylene (PE) fibers using radiation-induced graft polymerization (RIGP) provides a hydrophilic surface on the hydrophobic PE. When integrated with atom transfer radical polymerization (ATRP), the grafting of acrylonitrile (AN) and hydroxyethyl acrylate (HEA) can be controlled and manipulated more easily than with RIGP. Poly(acrylonitrile)-co-poly(hydroxyethyl acrylate) chains were grown via ATRP on PE-GMA fibers to generate an adsorbent for the extraction of uranium from seawater. The prepared adsorbents in this study demonstrated promise (159.9 g- U/kg of adsorbent) in laboratory screeningmore » tests using a high uranium concentration brine and 1.24 g-U/Kg of adsorbent in the filtered natural seawater in 21-days. The modest capacity in 21- days exceeds previous efforts to generate brush-on-brush adsorbents by ATRP while manipulating the apparent surface hydrophilicity of the trunk material (PE).« less