First-Principles Integrated Adsorption Modeling for Selective Capture of Uranium from Seawater by Polyamidoxime Sorbent Materials
Abstract
Nuclear power is a relatively carbon-free energy source that has the capacity to be utilized today in an effort to stem the tides of global warming. The growing demand for nuclear energy, however, could put significant strain on our uranium ore resources, and the mining activities utilized to extract that ore can leave behind long-term environmental damage. A potential solution to enhance the supply of uranium fuel is to recover uranium from seawater using amidoximated adsorbent fibers. This technology has been studied for decades but is currently plagued by the material’s relatively poor selectivity of uranium over its main competitor vanadium. In this work, we investigate the binding schemes between uranium, vanadium, and the amidoxime functional groups on the adsorbent surface. Using quantum chemical methods, binding strengths are approximated for a set of complexation reactions between uranium and vanadium with amidoxime functionalities. Those approximations are then coupled with a comprehensive aqueous adsorption model developed in this work to simulate the adsorption of uranium and vanadium under laboratory conditions. Experimental adsorption studies with uranium and vanadium over a wide pH range are performed, and the data collected are compared against simulation results to validate the model. It was found that couplingmore »
- Authors:
-
- Georgia Inst. of Technology, Atlanta, GA (United States)
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- Georgia Inst. of Technology, Atlanta, GA (United States); 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
- OSTI Identifier:
- 1436030
- Grant/Contract Number:
- AC05-00OR22725
- Resource Type:
- Accepted Manuscript
- Journal Name:
- ACS Applied Materials and Interfaces
- Additional Journal Information:
- Journal Volume: 10; Journal Issue: 15; Journal ID: ISSN 1944-8244
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; adsorption; amidoxime; modeling; uranium; vanadium
Citation Formats
Ladshaw, Austin P., Ivanov, Alexander S., Das, Sadananda, Bryantsev, Vyacheslav S., Tsouris, Costas, and Yiacoumi, Sotira. First-Principles Integrated Adsorption Modeling for Selective Capture of Uranium from Seawater by Polyamidoxime Sorbent Materials. United States: N. p., 2018.
Web. doi:10.1021/acsami.7b17031.
Ladshaw, Austin P., Ivanov, Alexander S., Das, Sadananda, Bryantsev, Vyacheslav S., Tsouris, Costas, & Yiacoumi, Sotira. First-Principles Integrated Adsorption Modeling for Selective Capture of Uranium from Seawater by Polyamidoxime Sorbent Materials. United States. https://doi.org/10.1021/acsami.7b17031
Ladshaw, Austin P., Ivanov, Alexander S., Das, Sadananda, Bryantsev, Vyacheslav S., Tsouris, Costas, and Yiacoumi, Sotira. Tue .
"First-Principles Integrated Adsorption Modeling for Selective Capture of Uranium from Seawater by Polyamidoxime Sorbent Materials". United States. https://doi.org/10.1021/acsami.7b17031. https://www.osti.gov/servlets/purl/1436030.
@article{osti_1436030,
title = {First-Principles Integrated Adsorption Modeling for Selective Capture of Uranium from Seawater by Polyamidoxime Sorbent Materials},
author = {Ladshaw, Austin P. and Ivanov, Alexander S. and Das, Sadananda and Bryantsev, Vyacheslav S. and Tsouris, Costas and Yiacoumi, Sotira},
abstractNote = {Nuclear power is a relatively carbon-free energy source that has the capacity to be utilized today in an effort to stem the tides of global warming. The growing demand for nuclear energy, however, could put significant strain on our uranium ore resources, and the mining activities utilized to extract that ore can leave behind long-term environmental damage. A potential solution to enhance the supply of uranium fuel is to recover uranium from seawater using amidoximated adsorbent fibers. This technology has been studied for decades but is currently plagued by the material’s relatively poor selectivity of uranium over its main competitor vanadium. In this work, we investigate the binding schemes between uranium, vanadium, and the amidoxime functional groups on the adsorbent surface. Using quantum chemical methods, binding strengths are approximated for a set of complexation reactions between uranium and vanadium with amidoxime functionalities. Those approximations are then coupled with a comprehensive aqueous adsorption model developed in this work to simulate the adsorption of uranium and vanadium under laboratory conditions. Experimental adsorption studies with uranium and vanadium over a wide pH range are performed, and the data collected are compared against simulation results to validate the model. It was found that coupling ab initio calculations with process level adsorption modeling provides accurate predictions of the adsorption capacity and selectivity of the sorbent materials. Furthermore, this work demonstrates that this multiscale modeling paradigm could be utilized to aid in the selection of superior ligands or ligand compositions for the selective capture of metal ions. Furthermore, this first-principles integrated modeling approach opens the door to the in silico design of next-generation adsorbents with potentially superior efficiency and selectivity for uranium over vanadium in seawater.},
doi = {10.1021/acsami.7b17031},
journal = {ACS Applied Materials and Interfaces},
number = 15,
volume = 10,
place = {United States},
year = {Tue Mar 27 00:00:00 EDT 2018},
month = {Tue Mar 27 00:00:00 EDT 2018}
}
Web of Science
Figures / Tables:
Works referenced in this record:
Extraction of Uranium from Sea Water
journal, September 1964
- Davies, R. V.; Kennedy, J.; McILROY, R. W.
- Nature, Vol. 203, Issue 4950
Actinide Carbonte Complexes and Their Importance in Actinide Environmental Chemistry
journal, January 1995
- Clark, David L.; Hobart, David E.; Neu, Mary P.
- Chemical Reviews, Vol. 95, Issue 1
Chemical Speciation of Uranium(VI) in Marine Environments: Complexation of Calcium and Magnesium Ions with [(UO 2 )(CO 3 ) 3 ] 4− and the Effect on the Extraction of Uranium from Seawater
journal, September 2014
- Endrizzi, Francesco; Rao, Linfeng
- Chemistry - A European Journal, Vol. 20, Issue 44
A comparison of three methods of determining the concentration of uranium in sea water
journal, January 1960
- Wilson, J. D.; Webster, R. K.; Milner, G. W. C.
- Analytica Chimica Acta, Vol. 23
Extraction of uranium from seawater by polymer-bound macrocyclic hexaketone
journal, August 1979
- Tabushi, Iwao; Kobuke, Yoshiaki; Nishiya, Takako
- Nature, Vol. 280, Issue 5724
Uranium recovery from industrial effluent by ion exchange—column experiments
journal, November 2005
- Ladeira, A. C. Q.; Morais, C. A.
- Minerals Engineering, Vol. 18, Issue 13-14, p. 1337-1340
Studies on membrane stability and recovery of uranium (VI) from aqueous solutions using a liquid emulsion membrane process
journal, April 2002
- Kulkarni, P. S.; Mukhopadhyay, S.; Bellary, M. P.
- Hydrometallurgy, Vol. 64, Issue 1
Determination of arsenic, molybdenum, uranium, and vanadium in seawater by by neutron activation analysis after preconcentration by colloid flotation
journal, April 1983
- Murthy, R. S. Shreedhara.; Ryan, Douglas E.
- Analytical Chemistry, Vol. 55, Issue 4
Adsorption and elution in hollow-fiber-packed bed for recovery of uranium from seawater
journal, January 1991
- Takeda, Toshiya; Saito, Kyoichi; Uezu, Kazuya
- Industrial & Engineering Chemistry Research, Vol. 30, Issue 1
Cost Estimation of Uranium Recovery from Seawater with System of Braid Type Adsorbent [モール状捕集システムによる海水ウラン捕集のコスト試算]
journal, January 2006
- Tamada, Masao; Seko, Noriaki; Kasai, Noboru
- Transactions of the Atomic Energy Society of Japan, Vol. 5, Issue 4
Present Status of Study on Extraction of Uranium from Sea Water
journal, January 1984
- Kanno, Masayoshi
- Journal of Nuclear Science and Technology, Vol. 21, Issue 1
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
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
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
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
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
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
Characteristics of uranium adsorption by amidoxime membrane synthesized by radiation-induced graft polymerization
journal, December 1987
- Saito, Kyoichi; Yamada, Shinji; Furusaki, Shintaro
- Journal of Membrane Science, Vol. 34, Issue 3
Density‐functional thermochemistry. III. The role of exact exchange
journal, April 1993
- Becke, Axel D.
- The Journal of Chemical Physics, Vol. 98, Issue 7, p. 5648-5652
Development of the Colle-Salvetti correlation-energy formula into a functional of the electron density
journal, January 1988
- Lee, Chengteh; Yang, Weitao; Parr, Robert G.
- Physical Review B, Vol. 37, Issue 2
The M06 suite of density functionals for main group thermochemistry, thermochemical kinetics, noncovalent interactions, excited states, and transition elements: two new functionals and systematic testing of four M06-class functionals and 12 other functionals
journal, July 2007
- Zhao, Yan; Truhlar, Donald G.
- Theoretical Chemistry Accounts, Vol. 120, Issue 1-3
Universal Solvation Model Based on Solute Electron Density and on a Continuum Model of the Solvent Defined by the Bulk Dielectric Constant and Atomic Surface Tensions
journal, May 2009
- Marenich, Aleksandr V.; Cramer, Christopher J.; Truhlar, Donald G.
- The Journal of Physical Chemistry B, Vol. 113, Issue 18, p. 6378-6396
Predicting Stability Constants for Uranyl Complexes Using Density Functional Theory
journal, March 2015
- Vukovic, Sinisa; Hay, Benjamin P.; Bryantsev, Vyacheslav S.
- Inorganic Chemistry, Vol. 54, Issue 8
Quantifying the binding strength of salicylaldoxime–uranyl complexes relative to competing salicylaldoxime–transition metal ion complexes in aqueous solution: a combined experimental and computational study
journal, January 2016
- Mehio, Nada; Ivanov, Alexander S.; Williams, Neil J.
- Dalton Transactions, Vol. 45, Issue 22
Assessing ligand selectivity for uranium over vanadium ions to aid in the discovery of superior adsorbents for extraction of UO 2 2+ from seawater
journal, January 2016
- Ivanov, Alexander S.; Bryantsev, Vyacheslav S.
- Dalton Transactions, Vol. 45, Issue 26
Experiments and Modeling of Uranium Uptake by Amidoxime-Based Adsorbent in the Presence of Other Ions in Simulated Seawater
journal, December 2015
- Ladshaw, A. P.; Das, S.; Liao, W. -P.
- Industrial & Engineering Chemistry Research, Vol. 55, Issue 15
MINEQL+: A software environment for chemical equilibrium modeling
journal, January 1992
- Schecher, William D.; McAvoy, Drew C.
- Computers, Environment and Urban Systems, Vol. 16, Issue 1
Statistical thermodynamics of liquid mixtures: A new expression for the excess Gibbs energy of partly or completely miscible systems
journal, January 1975
- Abrams, Denis S.; Prausnitz, John M.
- AIChE Journal, Vol. 21, Issue 1
An ion-binding model for ionic surfactant adsorption at aqueous-fluid interfaces
journal, August 1996
- Kalinin, V. V.; Radke, C. J.
- Colloids and Surfaces A: Physicochemical and Engineering Aspects, Vol. 114
Vacancy solution theory of adsorption using Flory-Huggins activity coefficient equations
journal, February 1985
- Cochran, T. W.; Kabel, R. L.; Danner, R. P.
- AIChE Journal, Vol. 31, Issue 2
Multicomponent adsorption equilibria of nonideal mixtures
journal, August 1986
- Talu, Orhan; Zwiebel, Imre
- AIChE Journal, Vol. 32, Issue 8
The Electrical Double Layer and the Theory of Electrocapillarity.
journal, December 1947
- Grahame, David C.
- Chemical Reviews, Vol. 41, Issue 3
van der Waals Volumes and Radii
journal, March 1964
- Bondi, A.
- The Journal of Physical Chemistry, Vol. 68, Issue 3, p. 441-451
Jacobian-free Newton–Krylov methods: a survey of approaches and applications
journal, January 2004
- Knoll, D. A.; Keyes, D. E.
- Journal of Computational Physics, Vol. 193, Issue 2
Development of Sorbers for the Recovery of Uranium from Seawater. Part 2. The Accumulation of Uranium from Seawater by Resins Containing Amidoxime and Imidoxime Functional Groups
journal, April 1983
- Astheimer, L.; Schenk, H. J.; Witte, E. G.
- Separation Science and Technology, Vol. 18, 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
Amidoximes as ligand functionalities for braided polymeric materials for the recovery of uranium from seawater
journal, April 2016
- Lashley, Mark A.; Mehio, Nada; Nugent, Joseph W.
- Polyhedron, Vol. 109
Sequestering uranium from seawater: binding strength and modes of uranyl complexes with glutarimidedioxime
journal, January 2012
- Tian, Guoxin; Teat, Simon J.; Zhang, Zhiyong
- Dalton Transactions, Vol. 41, Issue 38
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
Structural and spectroscopic studies of a rare non-oxido V( v ) complex crystallized from aqueous solution
journal, January 2016
- Leggett, C. J.; Parker, B. F.; Teat, S. J.
- Chemical Science, Vol. 7, Issue 4
Scientific Basis for Efficient Extraction of Uranium from Seawater, II: Fundamental Thermodynamic and Structural Studies
journal, December 2015
- Leggett, Christina J.; Endrizzi, Francesco; Rao, Linfeng
- Industrial & Engineering Chemistry Research, Vol. 55, Issue 15
Works referencing / citing this record:
3D hierarchical porous amidoxime fibers speed up uranium extraction from seawater
journal, January 2019
- Xu, Xiao; Zhang, Hongjun; Ao, Junxuan
- Energy & Environmental Science, Vol. 12, Issue 6
One-pot synthesis of multi-functional and environmental friendly tannic acid polymer with Fe3+ and formaldehyde as double crosslinking agents for selective removal of cation pollutants
journal, September 2019
- Zhang, Mingming; Zhang, Shengxiao; Liu, Xingxing
- Environmental Science and Pollution Research, Vol. 26, Issue 31
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
Predicting Stability Constants for Terbium(III) Complexes with Dipicolinic Acid and 4-Substituted Dipicolinic Acid Analogues using Density Functional Theory
journal, November 2019
- Chen, Hsieh; Shi, Rena; Ow, Hooisweng
- ACS Omega, Vol. 4, Issue 24
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
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