DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Extracting uranium from seawater: Promising AF series adsorbents

Abstract

Here, a new family of high surface area polyethylene fiber adsorbents (AF series) was recently developed at the Oak Ridge National Laboratory (ORNL). The AF series of were synthesized by radiation-induced graft polymerization of acrylonitrile and itaconic acid (at different monomer/co-monomer mol ratios) onto high surface area polyethylene fibers. The degree of grafting (%DOG) of AF series adsorbents was found to be 154 354%. The grafted nitrile groups were converted to amidoxime groups by treating with hydroxylamine. The amidoximated adsorbents were then conditioned with 0.44M KOH at 80 C followed by screening at ORNL with simulated seawater spiked with 8 ppm uranium. Uranium adsorption capacity in simulated seawater screening ranged from 170-200 g-U/kg-ads irrespective of %DOG. A monomer/co-monomer mol ratio in the range of 7.57-10.14 seemed to be optimum for highest uranium loading capacity. Subsequently, the adsorbents were also tested with natural seawater at Pacific Northwest National Laboratory (PNNL) using flow-through exposure uptake experiments to determine uranium loading capacity with varying KOH conditioning time at 80 C. The highest adsorption capacity of AF1 measured after 56 days of marine testing was demonstrated as 3.9 g-U/kg-adsorbent and 3.2 g-U/kg-adsorbent for 1hr and 3hrs of KOH conditioning at 80 C, respectively. Basedmore » on capacity values of several AF1 samples, it was observed that changing KOH conditioning from 3hrs to 1hr at 80 C resulted in 22-27% increase in uranium loading capacity in seawater.« less

Authors:
 [1];  [1];  [1];  [1];  [2];  [2];  [2];  [1]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  2. Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Publication Date:
Research Org.:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Nuclear Energy (NE)
OSTI Identifier:
1234340
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Industrial and Engineering Chemistry Research
Additional Journal Information:
Journal Volume: 55; Journal Issue: 15; Journal ID: ISSN 0888-5885
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
07 ISOTOPE AND RADIATION SOURCES; graft polymerization; amidoxime; uranium adsorption; seawater; KOH conditioning

Citation Formats

Das, Sadananda, Oyola, Y., Mayes, Richard T., Janke, Christopher James, Kuo, Li-Jung, Gill, Gary, Wood, Jordana, and Dai, Sheng. Extracting uranium from seawater: Promising AF series adsorbents. United States: N. p., 2015. Web. doi:10.1021/acs.iecr.5b03136.
Das, Sadananda, Oyola, Y., Mayes, Richard T., Janke, Christopher James, Kuo, Li-Jung, Gill, Gary, Wood, Jordana, & Dai, Sheng. Extracting uranium from seawater: Promising AF series adsorbents. United States. https://doi.org/10.1021/acs.iecr.5b03136
Das, Sadananda, Oyola, Y., Mayes, Richard T., Janke, Christopher James, Kuo, Li-Jung, Gill, Gary, Wood, Jordana, and Dai, Sheng. Mon . "Extracting uranium from seawater: Promising AF series adsorbents". United States. https://doi.org/10.1021/acs.iecr.5b03136. https://www.osti.gov/servlets/purl/1234340.
@article{osti_1234340,
title = {Extracting uranium from seawater: Promising AF series adsorbents},
author = {Das, Sadananda and Oyola, Y. and Mayes, Richard T. and Janke, Christopher James and Kuo, Li-Jung and Gill, Gary and Wood, Jordana and Dai, Sheng},
abstractNote = {Here, a new family of high surface area polyethylene fiber adsorbents (AF series) was recently developed at the Oak Ridge National Laboratory (ORNL). The AF series of were synthesized by radiation-induced graft polymerization of acrylonitrile and itaconic acid (at different monomer/co-monomer mol ratios) onto high surface area polyethylene fibers. The degree of grafting (%DOG) of AF series adsorbents was found to be 154 354%. The grafted nitrile groups were converted to amidoxime groups by treating with hydroxylamine. The amidoximated adsorbents were then conditioned with 0.44M KOH at 80 C followed by screening at ORNL with simulated seawater spiked with 8 ppm uranium. Uranium adsorption capacity in simulated seawater screening ranged from 170-200 g-U/kg-ads irrespective of %DOG. A monomer/co-monomer mol ratio in the range of 7.57-10.14 seemed to be optimum for highest uranium loading capacity. Subsequently, the adsorbents were also tested with natural seawater at Pacific Northwest National Laboratory (PNNL) using flow-through exposure uptake experiments to determine uranium loading capacity with varying KOH conditioning time at 80 C. The highest adsorption capacity of AF1 measured after 56 days of marine testing was demonstrated as 3.9 g-U/kg-adsorbent and 3.2 g-U/kg-adsorbent for 1hr and 3hrs of KOH conditioning at 80 C, respectively. Based on capacity values of several AF1 samples, it was observed that changing KOH conditioning from 3hrs to 1hr at 80 C resulted in 22-27% increase in uranium loading capacity in seawater.},
doi = {10.1021/acs.iecr.5b03136},
journal = {Industrial and Engineering Chemistry Research},
number = 15,
volume = 55,
place = {United States},
year = {Mon Nov 02 00:00:00 EST 2015},
month = {Mon Nov 02 00:00:00 EST 2015}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Citation Metrics:
Cited by: 112 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

Spectrophotometric determination of uranium in sea water after extraction with aliquat-336
journal, January 1978


Adsorption equilibrium of uranium from aqueous [UO2(CO3)3]4? solutions on a polymer bearing amidoxime groups
journal, January 1986

  • Hirotsu, Takahiro; Katoh, Shunsaku; Sugasaka, Kazuhiko
  • Journal of the Chemical Society, Dalton Transactions, Issue 9
  • DOI: 10.1039/dt9860001983

Synthesis and characterization of a novel graft copolymer containing carboxyl groups and its application to extract uranium(VI) from aqueous media
journal, May 2011

  • Anirudhan, Thayyath S.; Tharun, Abdul R.; Rijith, Sreenivasan
  • Journal of Applied Polymer Science, Vol. 122, Issue 2
  • DOI: 10.1002/app.34126

The adsorption mechanism of uranium(VI) from seawater on a macroporous fibrous polymeric adsorbent containing amidoxime chelating functional group
journal, November 2003


Determination of uranium(VI) in natural waters after preconcentration on adsorbent containing m-aminophenol fragments
journal, January 2013

  • Basargin, N. N.; Magerramov, A. M.; Gadzhieva, S. R.
  • Journal of Analytical Chemistry, Vol. 68, Issue 2
  • DOI: 10.1134/S1061934813020032

Extraction of Uranium from Sea Water
journal, September 1964

  • Davies, R. V.; Kennedy, J.; McILROY, R. W.
  • Nature, Vol. 203, Issue 4950
  • DOI: 10.1038/2031110a0

Status of Technology for the Recovery of Uranium from Seawater
journal, October 1981


Complex-forming polymer prepared by electron beam radiation-induced graft polymerization
journal, January 1985


Development of Sorbers for the Recovery of Uranium from Seawater. 1. Assessment of Key Parameters and Screening Studies of Sorber Materials
journal, August 1982

  • Schenk, H. J.; Astheimer, L.; Witte, E. G.
  • Separation Science and Technology, Vol. 17, Issue 11
  • DOI: 10.1080/01496398208056103

Sorption of uranium(VI) from aqueous solution onto magnesium silicate hollow spheres
journal, April 2011

  • Fan, Fangli; Ding, Huajie; Bai, Jing
  • Journal of Radioanalytical and Nuclear Chemistry, Vol. 289, Issue 2
  • DOI: 10.1007/s10967-011-1091-1

Adsorption of uranium ions by resins with amidoxime and amidoxime/carboxyl group prepared by radiation-induced polymerization
journal, June 2003


Adsorption of uranium(VI) onto Ulva sp.-sepiolite composite
journal, July 2008

  • Donat, R.; Esen, K.; Cetisli, H.
  • Journal of Radioanalytical and Nuclear Chemistry, Vol. 279, Issue 1
  • DOI: 10.1007/s10967-007-7243-7

Uptake of Uranium from Seawater by Amidoxime-Based Polymeric Adsorbent: Field Experiments, Modeling, and Updated Economic Assessment
journal, March 2014

  • Kim, Jungseung; Tsouris, Costas; Oyola, Yatsandra
  • Industrial & Engineering Chemistry Research, Vol. 53, Issue 14
  • DOI: 10.1021/ie4039828

Characterization of Uranium Uptake Kinetics from Seawater in Batch and Flow-Through Experiments
journal, June 2013

  • Kim, Jungseung; Oyola, Yatsandra; Tsouris, Costas
  • Industrial & Engineering Chemistry Research, Vol. 52, Issue 27
  • DOI: 10.1021/ie400587f

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


Uranium recovery from seawater: development of fiber adsorbents prepared via atom-transfer radical polymerization
journal, January 2014

  • Saito, Tomonori; Brown, Suree; Chatterjee, Sabornie
  • J. Mater. Chem. A, Vol. 2, Issue 35
  • DOI: 10.1039/C4TA03276D

Macroporous monoliths for trace metal extraction from seawater
journal, January 2015

  • Yue, Yanfeng; Mayes, Richard T.; Gill, Gary
  • RSC Advances, Vol. 5, Issue 62
  • DOI: 10.1039/C5RA02131F

Predicting Stability Constants for Uranyl Complexes Using Density Functional Theory
journal, March 2015


Development of a Kelp-Type Structure Module in a Coastal Ocean Model to Assess the Hydrodynamic Impact of Seawater Uranium Extraction Technology
journal, February 2014

  • Wang, Taiping; Khangaonkar, Tarang; Long, Wen
  • Journal of Marine Science and Engineering, Vol. 2, Issue 1
  • DOI: 10.3390/jmse2010081

Complexation of uranium( vi ) with glutarimidoxioxime: thermodynamic and computational studies
journal, January 2015

  • Endrizzi, Francesco; Melchior, Andrea; Tolazzi, Marilena
  • Dalton Transactions, Vol. 44, Issue 31
  • DOI: 10.1039/C5DT00261C

Acidity of the Amidoxime Functional Group in Aqueous Solution: A Combined Experimental and Computational Study
journal, February 2015

  • Mehio, Nada; Lashely, Mark A.; Nugent, Joseph W.
  • The Journal of Physical Chemistry B, Vol. 119, Issue 8
  • DOI: 10.1021/jp512778x

Quantifying the binding strength of U( vi ) with phthalimidedioxime in comparison with glutarimidedioxime
journal, January 2014

  • Sun, Xiaoqi; Tian, Guoxin; Xu, Chao
  • Dalton Trans., Vol. 43, Issue 2
  • DOI: 10.1039/C3DT52206G

Structural clues to UO 2 2+ /VO 2 + competition in seawater extraction using amidoxime-based extractants
journal, January 2014

  • Kelley, Steven P.; Barber, Patrick S.; Mullins, Peter H. K.
  • Chem. Commun., Vol. 50, Issue 83
  • DOI: 10.1039/C4CC06370H

Biomimetic Mineralization of Uranium by Metabolically-Inactive Shrimp Shell
journal, October 2014

  • Griggs, C. S.; Barber, P. S.; Kelley, S. P.
  • Crystal Growth & Design, Vol. 14, Issue 12
  • DOI: 10.1021/cg5015576

Adsorption of Trace Heavy Metals:  Application of Surface Complexation Theory to a Macroporous Polymer and a Weakly Acidic Ion-Exchange Resin
journal, February 2005

  • Saha, B.; Streat, M.
  • Industrial & Engineering Chemistry Research, Vol. 44, Issue 23
  • DOI: 10.1021/ie048848+

γ-Induced Graft Copolymerization onto Cellulosic Fabric Waste for Cationic Dye Removal
journal, July 2005


Vanadium speciation and cycling in coastal waters
journal, December 2009


Fractional Elution and Determination of Uranium and Vanadium Adsorbed on Amidoxime Fiber from Seawater.
journal, January 2000

  • Suzuki, Toshihiro; Saito, Kyoichi; Sugo, Takanobu
  • Analytical Sciences, Vol. 16, Issue 4
  • DOI: 10.2116/analsci.16.429

Exchanges of Uranium(VI) Species in Amidoxime-Functionalized Sorbents
journal, April 2009

  • Das, Sadananda; Pandey, Ashok K.; Athawale, Anjali A.
  • The Journal of Physical Chemistry B, Vol. 113, Issue 18
  • DOI: 10.1021/jp8097928

Comparison of Amidoxime Adsorbents Prepared by Cografting Methacrylic Acid and 2-Hydroxyethyl Methacrylate with Acrylonitrile onto Polyethylene
journal, August 2000

  • Kawai, Tomomi; Saito, Kyoichi; Sugita, Kazuyuki
  • Industrial & Engineering Chemistry Research, Vol. 39, Issue 8
  • DOI: 10.1021/ie990474a

Effect of seawater temperature on uranium recovery from seawater using amidoxime adsorbents
journal, March 1994

  • Sekiguchi, Koji; Saito, Kyoichi; Konishi, Satoshi
  • Industrial & Engineering Chemistry Research, Vol. 33, Issue 3
  • DOI: 10.1021/ie00027a025

Adsorptive Preconcentration of Uranium in Hydrogels from Seawater and Aqueous Solutions
journal, July 2009

  • Das, Sadananda; Pandey, Ashok K.; Vasudevan, T.
  • Industrial & Engineering Chemistry Research, Vol. 48, Issue 14
  • DOI: 10.1021/ie801912n

Cyclic Imide Dioximes: Formation and Hydrolytic Stability
journal, May 2012

  • Kang, Sung Ok; Vukovic, Sinisa; Custelcean, Radu
  • Industrial & Engineering Chemistry Research, Vol. 51, Issue 19
  • DOI: 10.1021/ie300492z

Enhancing Uranium Uptake by Amidoxime Adsorbent in Seawater: An Investigation for Optimum Alkaline Conditioning Parameters
journal, September 2015

  • Das, S.; Tsouris, C.; Zhang, C.
  • Industrial & Engineering Chemistry Research, Vol. 55, Issue 15
  • DOI: 10.1021/acs.iecr.5b02735

Works referencing / citing this record:

Fit-for-purpose block polymer membranes molecularly engineered for water treatment
journal, April 2018

  • Zhang, Yizhou; Almodovar-Arbelo, Noelia E.; Weidman, Jacob L.
  • npj Clean Water, Vol. 1, Issue 1
  • DOI: 10.1038/s41545-018-0002-1

Polyamidoxime chain length drives emergent metal-binding phenomena
journal, January 2019

  • Earl, L. D.; Do, C.; Wang, Y.
  • Physical Chemistry Chemical Physics, Vol. 21, Issue 2
  • DOI: 10.1039/c8cp02198h

Ultrafast and Highly Selective Uranium Extraction from Seawater by Hydrogel-like Spidroin-based Protein Fiber
journal, July 2019

  • Yuan, Yihui; Yu, Qiuhan; Wen, Jun
  • Angewandte Chemie International Edition, Vol. 58, Issue 34
  • DOI: 10.1002/anie.201906191

Functional polymer brushes for highly efficient extraction of uranium from seawater
journal, October 2018


Engineering robust metal–phenolic network membranes for uranium extraction from seawater
journal, January 2019

  • Luo, Wei; Xiao, Gao; Tian, Fan
  • Energy & Environmental Science, Vol. 12, Issue 2
  • DOI: 10.1039/c8ee01438h

Photoinduced Multiple Effects to Enhance Uranium Extraction from Natural Seawater by Black Phosphorus Nanosheets
journal, December 2019

  • Yuan, Yihui; Niu, Biye; Yu, Qiuhan
  • Angewandte Chemie International Edition, Vol. 59, Issue 3
  • DOI: 10.1002/anie.201913644

Significantly Enhanced Uranium Extraction from Seawater with Mass Produced Fully Amidoximated Nanofiber Adsorbent
journal, October 2018


Ultrafast and Highly Selective Uranium Extraction from Seawater by Hydrogel‐like Spidroin‐based Protein Fiber
journal, July 2019


Rational Design of Porous Nanofiber Adsorbent by Blow-Spinning with Ultrahigh Uranium Recovery Capacity from Seawater
journal, November 2018

  • Yuan, Yihui; Zhao, Shilei; Wen, Jun
  • Advanced Functional Materials, Vol. 29, Issue 2
  • DOI: 10.1002/adfm.201805380

Origin of the unusually strong and selective binding of vanadium by polyamidoximes in seawater
journal, November 2017

  • Ivanov, Alexander S.; Leggett, Christina J.; Parker, Bernard F.
  • Nature Communications, Vol. 8, Issue 1
  • DOI: 10.1038/s41467-017-01443-1

Photoinduced Multiple Effects to Enhance Uranium Extraction from Natural Seawater by Black Phosphorus Nanosheets
journal, November 2019


A Dual‐Surface Amidoximated Halloysite Nanotube for High‐Efficiency Economical Uranium Extraction from Seawater
journal, September 2019

  • Zhao, Shilei; Yuan, Yihui; Yu, Qiuhan
  • Angewandte Chemie International Edition, Vol. 58, Issue 42
  • DOI: 10.1002/anie.201908762

A Dual‐Surface Amidoximated Halloysite Nanotube for High‐Efficiency Economical Uranium Extraction from Seawater
journal, September 2019


Amidoxime Polymers for Uranium Adsorption: Influence of Comonomers and Temperature
journal, November 2017

  • Ladshaw, Austin P.; Wiechert, Alexander I.; Das, Sadananda
  • Materials, Vol. 10, Issue 11
  • DOI: 10.3390/ma10111268

A Marine‐Inspired Hybrid Sponge for Highly Efficient Uranium Extraction from Seawater
journal, May 2019

  • Wang, Dong; Song, Jianan; Lin, Sen
  • Advanced Functional Materials, Vol. 29, Issue 32
  • DOI: 10.1002/adfm.201901009

A highly efficient uranium grabber derived from acrylic fiber for extracting uranium from seawater
journal, January 2020

  • Pan, Horng-Bin; Wai, Chien M.; Kuo, Li-Jung
  • Dalton Transactions, Vol. 49, Issue 9
  • DOI: 10.1039/c9dt04562g

The use of silver nanoparticles for the recovery of uranium from seawater by means of biofouling mitigation
journal, January 2018

  • Byers, Margaret Flicker; Landsberger, Sheldon; Schneider, Erich
  • Sustainable Energy & Fuels, Vol. 2, Issue 10
  • DOI: 10.1039/c8se00228b

Amidoxime Polymers for Uranium Adsorption: Influence of Comonomers and Temperature
journal, November 2017

  • Ladshaw, Austin P.; Wiechert, Alexander I.; Das, Sadananda
  • Materials, Vol. 10, Issue 11
  • DOI: 10.3390/ma10111268