Investigations into the Reusability of Amidoxime-Based Polymeric Adsorbents for Seawater Uranium Extraction
Abstract
The ability to reuse amidoxime-based polymeric adsorbents is a critical component in reducing the overall cost of the technology to extract uranium from seawater. This paper describes an evaluation of adsorbent reusability in multiple reuse (adsorption/stripping) cycles in real seawater exposures with potassium bicarbonate (KHCO3) elution using several amidoxime-based polymeric adsorbents. The KHCO3 elution technique achieved ~100% recovery of uranium adsorption capacity in the first reuse. Subsequent reuses showed significant drops in adsorption capacity. After the fourth reuse with the ORNL AI8 adsorbent, the 56-day adsorption capacity dropped to 28% of its original capacity. FTIR spectra revealed that there was a conversion of the amidoxime ligands to carboxylate groups during extended seawater exposure, becoming more significant with longer exposure times. Ca and Mg adsorption capacities also increased with each reuse cycle supporting the hypothesis that long-term exposure resulted in converting amidoxime to carboxylate, enhancing the adsorption of Ca and Mg. Shorter seawater exposure (adsorption/stripping) cycles (28 vs 42 days) had higher adsorption capacities after reuse, but the shorter exposure cycle time did not produce an overall better performance in terms of cumulative exposure time. Recovery of uranium capacity in reuses may also vary across different adsorbent formulations. Through multiple reuses,more »
- Authors:
-
- Pacific Northwest National Lab. (PNNL), Sequim, WA (United States). Marine Sciences Lab.
- Univ. of Idaho, Moscow, ID (United States). Dept. of Chemistry
- Univ. of Texas, Austin, TX (United States). Nuclear and Radiation Engineering Program
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- Publication Date:
- Research Org.:
- Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
- Sponsoring Org.:
- USDOE Office of Nuclear Energy (NE), Fuel Cycle Technologies (NE-5)
- OSTI Identifier:
- 1471881
- Grant/Contract Number:
- AC05-00OR22725; AC05-76RL01830
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Industrial and Engineering Chemistry Research
- Additional Journal Information:
- Journal Volume: 56; Journal Issue: 40; Journal ID: ISSN 0888-5885
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEAR CHEMISTRY
Citation Formats
Kuo, Li-Jung, Pan, Horng-Bin, Wai, Chien M., Byers, Margaret F., Schneider, Erich, Strivens, Jonathan E., Janke, Christopher J., Das, Sadananda, Mayes, Richard T., Wood, Jordana R., Schlafer, Nicholas, and Gill, Gary A. Investigations into the Reusability of Amidoxime-Based Polymeric Adsorbents for Seawater Uranium Extraction. United States: N. p., 2017.
Web. doi:10.1021/acs.iecr.7b02893.
Kuo, Li-Jung, Pan, Horng-Bin, Wai, Chien M., Byers, Margaret F., Schneider, Erich, Strivens, Jonathan E., Janke, Christopher J., Das, Sadananda, Mayes, Richard T., Wood, Jordana R., Schlafer, Nicholas, & Gill, Gary A. Investigations into the Reusability of Amidoxime-Based Polymeric Adsorbents for Seawater Uranium Extraction. United States. https://doi.org/10.1021/acs.iecr.7b02893
Kuo, Li-Jung, Pan, Horng-Bin, Wai, Chien M., Byers, Margaret F., Schneider, Erich, Strivens, Jonathan E., Janke, Christopher J., Das, Sadananda, Mayes, Richard T., Wood, Jordana R., Schlafer, Nicholas, and Gill, Gary A. Wed .
"Investigations into the Reusability of Amidoxime-Based Polymeric Adsorbents for Seawater Uranium Extraction". United States. https://doi.org/10.1021/acs.iecr.7b02893. https://www.osti.gov/servlets/purl/1471881.
@article{osti_1471881,
title = {Investigations into the Reusability of Amidoxime-Based Polymeric Adsorbents for Seawater Uranium Extraction},
author = {Kuo, Li-Jung and Pan, Horng-Bin and Wai, Chien M. and Byers, Margaret F. and Schneider, Erich and Strivens, Jonathan E. and Janke, Christopher J. and Das, Sadananda and Mayes, Richard T. and Wood, Jordana R. and Schlafer, Nicholas and Gill, Gary A.},
abstractNote = {The ability to reuse amidoxime-based polymeric adsorbents is a critical component in reducing the overall cost of the technology to extract uranium from seawater. This paper describes an evaluation of adsorbent reusability in multiple reuse (adsorption/stripping) cycles in real seawater exposures with potassium bicarbonate (KHCO3) elution using several amidoxime-based polymeric adsorbents. The KHCO3 elution technique achieved ~100% recovery of uranium adsorption capacity in the first reuse. Subsequent reuses showed significant drops in adsorption capacity. After the fourth reuse with the ORNL AI8 adsorbent, the 56-day adsorption capacity dropped to 28% of its original capacity. FTIR spectra revealed that there was a conversion of the amidoxime ligands to carboxylate groups during extended seawater exposure, becoming more significant with longer exposure times. Ca and Mg adsorption capacities also increased with each reuse cycle supporting the hypothesis that long-term exposure resulted in converting amidoxime to carboxylate, enhancing the adsorption of Ca and Mg. Shorter seawater exposure (adsorption/stripping) cycles (28 vs 42 days) had higher adsorption capacities after reuse, but the shorter exposure cycle time did not produce an overall better performance in terms of cumulative exposure time. Recovery of uranium capacity in reuses may also vary across different adsorbent formulations. Through multiple reuses, the AI8 adsorbent can harvest 10 g uranium/kg adsorbent in ~140 days, using a 28-day adsorption/stripping cycle, a performance much better than would be achieved with a single use of the adsorbent through a very long-term exposure (saturation capacity of 7.4 g U/kg adsorbent). A time dependent seawater exposure model to evaluate the cost associated with reusing amidoxime-based adsorbents in real seawater exposures was developed. The predicted cost to extract uranium from seawater ranged from $610/kg U to 830/kg U. Finally, model simulation suggests that a short seawater exposure cycle (<15 days) is the optimal deployment period for lower uranium production cost in seawater uranium mining.},
doi = {10.1021/acs.iecr.7b02893},
journal = {Industrial and Engineering Chemistry Research},
number = 40,
volume = 56,
place = {United States},
year = {Wed Sep 13 00:00:00 EDT 2017},
month = {Wed Sep 13 00:00:00 EDT 2017}
}
Web of Science
Works referenced in this record:
Bicarbonate Elution of Uranium from Amidoxime-Based Polymer Adsorbents for Sequestering Uranium from Seawater
journal, May 2017
- Pan, Horng-Bin; Wai, Chien M.; Kuo, Li-Jung
- ChemistrySelect, Vol. 2, Issue 13
Novel poly(imide dioxime) sorbents: Development and testing for enhanced extraction of uranium from natural seawater
journal, August 2016
- Das, S.; Brown, S.; Mayes, R. T.
- Chemical Engineering Journal, Vol. 298
The Uranium from Seawater Program at the Pacific Northwest National Laboratory: Overview of Marine Testing, Adsorbent Characterization, Adsorbent Durability, Adsorbent Toxicity, and Deployment Studies
journal, December 2015
- Gill, Gary A.; Kuo, Li-Jung; Janke, Chris J.
- Industrial & Engineering Chemistry Research, Vol. 55, Issue 15
Elution of Uranium and Transition Metals from Amidoxime-Based Polymer Adsorbents for Sequestering Uranium from Seawater
journal, December 2015
- Pan, Horng-Bin; Kuo, Li-Jung; Wai, Chien M.
- Industrial & Engineering Chemistry Research, Vol. 55, Issue 15
Recovery System for Uranium from Seawater with Fibrous Adsorbent and Its Preliminary Cost Estimation. [海水ウラン捕集のコスト評価と実用化に向けての技術課題]
journal, January 2001
- Sugo, Takanobu; Tamada, Masao; Seguchi, Tadao
- Journal of the Atomic Energy Society of Japan / Atomic Energy Society of Japan, Vol. 43, Issue 10
Electrospun nanofibrous adsorbents for uranium extraction from seawater
journal, January 2015
- Xie, Siyuan; Liu, Xiyan; Zhang, Bowu
- Journal of Materials Chemistry A, Vol. 3, Issue 6
Sources and reactions of OH and daughter radicals in seawater
journal, October 1974
- Zafiriou, Oliver C.
- Journal of Geophysical Research, Vol. 79, Issue 30
Characterization and Testing of Amidoxime-Based Adsorbent Materials to Extract Uranium from Natural Seawater
journal, December 2015
- Kuo, Li-Jung; Janke, Christopher J.; Wood, Jordana R.
- Industrial & Engineering Chemistry Research, Vol. 55, Issue 15
Halogen radicals contribute to photooxidation in coastal and estuarine waters
journal, May 2016
- Parker, Kimberly M.; Mitch, William A.
- Proceedings of the National Academy of Sciences, Vol. 113, Issue 21
Optimization of the Passive Recovery of Uranium from Seawater
journal, December 2015
- Flicker Byers, M.; Schneider, E.
- Industrial & Engineering Chemistry Research, Vol. 55, Issue 15
The Cost of Recovering Uranium from Seawater by a Braided Polymer Adsorbent System
journal, May 2013
- Schneider, Erich; Sachde, Darshan
- Science & Global Security, Vol. 21, Issue 2
Recovery of Uranium from Seawater: A Review of Current Status and Future Research Needs
journal, January 2013
- Kim, Jungseung; Tsouris, Costas; Mayes, Richard T.
- Separation Science and Technology, Vol. 48, Issue 3
Extracting Uranium from Seawater: Promising AF Series Adsorbents
journal, November 2015
- Das, S.; Oyola, Y.; Mayes, Richard T.
- Industrial & Engineering Chemistry Research, Vol. 55, Issue 15
Uranium Adsorbent Fibers Prepared by Atom-Transfer Radical Polymerization (ATRP) from Poly(vinyl chloride)- co -chlorinated Poly(vinyl chloride) (PVC- co -CPVC) Fiber
journal, December 2015
- Brown, Suree; Yue, Yanfeng; Kuo, Li-Jung
- Industrial & Engineering Chemistry Research, Vol. 55, Issue 15
Extracting Uranium from Seawater: Promising AI Series Adsorbents
journal, November 2015
- Das, S.; Oyola, Y.; Mayes, R. T.
- Industrial & Engineering Chemistry Research, Vol. 55, Issue 15
Building future nuclear power fleets: The available uranium resources constraint
journal, December 2013
- Gabriel, Sophie; Baschwitz, Anne; Mathonnière, Gilles
- Resources Policy, Vol. 38, Issue 4
Uranium extraction: Fuel from seawater
journal, February 2017
- Tsouris, Costas
- Nature Energy, Vol. 2, Issue 4
Fine Fibrous Amidoxime Adsorbent Synthesized by Grafting and Uranium Adsorption–Elution Cyclic Test with Seawater
journal, January 2004
- Seko, Noriaki; Katakai, Akio; Tamada, Masao
- Separation Science and Technology, Vol. 39, Issue 16
Effect of Biofouling on the Performance of Amidoxime-Based Polymeric Uranium Adsorbents
journal, December 2015
- Park, Jiyeon; Gill, Gary A.; Strivens, Jonathan E.
- Industrial & Engineering Chemistry Research, Vol. 55, Issue 15
Carbonate–H 2 O 2 leaching for sequestering uranium from seawater
journal, January 2014
- Pan, Horng-Bin; Liao, Weisheng; Wai, Chien M.
- Dalton Trans., Vol. 43, Issue 28
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
Review of cost estimates for uranium recovery from seawater
journal, May 2015
- Lindner, Harry; Schneider, Erich
- Energy Economics, Vol. 49
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
Towards understanding KOH conditioning of amidoxime-based polymer adsorbents for sequestering uranium from seawater
journal, January 2015
- Pan, Horng-Bin; Kuo, Li-Jung; Wood, Jordana
- RSC Advances, Vol. 5, Issue 122
Recovery of uranium from seawater. 13. Long-term stability tests for high-performance chelating resins containing amidoxime groups and evaluation of elution process
journal, March 1993
- Egawa, Hiroaki; Kabay, Nalan; Shuto, Taketomi
- Industrial & Engineering Chemistry Research, Vol. 32, Issue 3
Polyoxime-functionalized magnetic nanoparticles for uranium adsorption with high selectivity over vanadium
journal, January 2017
- Xu, Meiyun; Han, Xiaoli; Hua, Daoben
- Journal of Materials Chemistry A, Vol. 5, Issue 24
Current Status of Technology for Collection of Uranium from Seawater
conference, January 2012
- Tamada, Masao
- International Seminar on Nuclear War and Planetary Emergencies 42nd Session, International Seminar on Nuclear War and Planetary Emergencies — 42nd Session
Works referencing / citing this record:
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
Siderophore-inspired chelator hijacks uranium from aqueous medium
journal, February 2019
- Ivanov, Alexander S.; Parker, Bernard F.; Zhang, Zhicheng
- Nature Communications, Vol. 10, Issue 1
Symbiotic Aerogel Fibers Made via In-Situ Gelation of Aramid Nanofibers with Polyamidoxime for Uranium Extraction
journal, May 2019
- Li, Juan; Wang, Jin; Wang, Wei
- Molecules, Vol. 24, Issue 9
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
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
Siderophore-inspired chelator hijacks uranium from aqueous medium
journal, February 2019
- Ivanov, Alexander S.; Parker, Bernard F.; Zhang, Zhicheng
- Nature Communications, Vol. 10, Issue 1
Symbiotic Aerogel Fibers Made via In-Situ Gelation of Aramid Nanofibers with Polyamidoxime for Uranium Extraction
journal, May 2019
- Li, Juan; Wang, Jin; Wang, Wei
- Molecules, Vol. 24, Issue 9