Assessing ligand selectivity for uranium over vanadium ions to aid in the discovery of superior adsorbents for extraction of UO22+ from seawater
Abstract
Uranium is used as the basic fuel for nuclear power plants, which generate significant amounts of electricity and have life cycle carbon emissions that are as low as renewable energy sources. However, the extraction of this valuable energy commodity from the ground remains controversial, mainly because of environmental and health impacts. Alternatively, seawater offers an enormous uranium resource that may be tapped at minimal environmental cost. Nowadays, amidoxime polymers are the most widely utilized sorbent materials for large-scale extraction of uranium from seawater, but they are not perfectly selective for uranyl, UO22+. In particular, the competition between UO22+ and VO2+/VO2+ cations poses a significant challenge to the effi-cient mining of UO22+. Thus, screening and rational design of more selective ligands must be accomplished. One of the key components in achieving this goal is the establishment of computational techniques capable of assessing ligand selec-tivity trends. Here, we report an approach based on quantum chemical calculations that achieves high accuracy in repro-ducing experimental aqueous stability constants for VO2+/VO2+ complexes with ten different oxygen donor lig-ands. The predictive power of the developed computational protocol was demonstrated for amidoxime-type ligands, providing greater insights into new design strategies for the development of the next generationmore »
- Authors:
-
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- Publication Date:
- Research Org.:
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- Sponsoring Org.:
- USDOE Office of Nuclear Energy (NE)
- OSTI Identifier:
- 1331080
- Grant/Contract Number:
- AC05-00OR22725
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Dalton Transactions
- Additional Journal Information:
- Journal Volume: 45; Journal Issue: 26; Journal ID: ISSN 1477-9226
- Publisher:
- Royal Society of Chemistry
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 07 ISOTOPE AND RADIATION SOURCES; 54 ENVIRONMENTAL SCIENCES
Citation Formats
Ivanov, Alexander S., and Bryantsev, Vyacheslav S. Assessing ligand selectivity for uranium over vanadium ions to aid in the discovery of superior adsorbents for extraction of UO22+ from seawater. United States: N. p., 2016.
Web. doi:10.1039/C6DT01752E.
Ivanov, Alexander S., & Bryantsev, Vyacheslav S. Assessing ligand selectivity for uranium over vanadium ions to aid in the discovery of superior adsorbents for extraction of UO22+ from seawater. United States. https://doi.org/10.1039/C6DT01752E
Ivanov, Alexander S., and Bryantsev, Vyacheslav S. Mon .
"Assessing ligand selectivity for uranium over vanadium ions to aid in the discovery of superior adsorbents for extraction of UO22+ from seawater". United States. https://doi.org/10.1039/C6DT01752E. https://www.osti.gov/servlets/purl/1331080.
@article{osti_1331080,
title = {Assessing ligand selectivity for uranium over vanadium ions to aid in the discovery of superior adsorbents for extraction of UO22+ from seawater},
author = {Ivanov, Alexander S. and Bryantsev, Vyacheslav S.},
abstractNote = {Uranium is used as the basic fuel for nuclear power plants, which generate significant amounts of electricity and have life cycle carbon emissions that are as low as renewable energy sources. However, the extraction of this valuable energy commodity from the ground remains controversial, mainly because of environmental and health impacts. Alternatively, seawater offers an enormous uranium resource that may be tapped at minimal environmental cost. Nowadays, amidoxime polymers are the most widely utilized sorbent materials for large-scale extraction of uranium from seawater, but they are not perfectly selective for uranyl, UO22+. In particular, the competition between UO22+ and VO2+/VO2+ cations poses a significant challenge to the effi-cient mining of UO22+. Thus, screening and rational design of more selective ligands must be accomplished. One of the key components in achieving this goal is the establishment of computational techniques capable of assessing ligand selec-tivity trends. Here, we report an approach based on quantum chemical calculations that achieves high accuracy in repro-ducing experimental aqueous stability constants for VO2+/VO2+ complexes with ten different oxygen donor lig-ands. The predictive power of the developed computational protocol was demonstrated for amidoxime-type ligands, providing greater insights into new design strategies for the development of the next generation of adsorbents with high selectivity toward UO22+over VO2+/VO2+ ions. Furthermore, the results of calculations suggest that alkylation of amidox-ime moieties present in poly(acrylamidoxime) sorbents can be a potential route to better discrimination between the uranyl and competing vanadium ions within seawater.},
doi = {10.1039/C6DT01752E},
journal = {Dalton Transactions},
number = 26,
volume = 45,
place = {United States},
year = {Mon Jun 06 00:00:00 EDT 2016},
month = {Mon Jun 06 00:00:00 EDT 2016}
}
Free Publicly Available Full Text
Publisher's Version of Record
Other availability
Search WorldCat to find libraries that may hold this journal
Cited by: 19 works
Citation information provided by
Web of Science
Web of Science
Save to My Library
You must Sign In or Create an Account in order to save documents to your library.
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
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
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
How Amidoximate Binds the Uranyl Cation
journal, February 2012
- Vukovic, Sinisa; Watson, Lori A.; Kang, Sung Ok
- Inorganic Chemistry, Vol. 51, Issue 6
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
De Novo Structure-Based Design of Bis-amidoxime Uranophiles
journal, June 2013
- Vukovic, Sinisa; Hay, Benjamin P.
- Inorganic Chemistry, Vol. 52, Issue 13
Theoretical studies on the complexation of uranyl with typical carboxylate and amidoximate ligands
journal, October 2013
- Xu, ChaoFei; Su, Jing; Xu, Xiang
- Science China Chemistry, Vol. 56, Issue 11
Theoretical Insights on the Interaction of Uranium with Amidoxime and Carboxyl Groups
journal, August 2014
- Wang, Cong-Zhi; Lan, Jian-Hui; Wu, Qun-Yan
- Inorganic Chemistry, Vol. 53, Issue 18
Tuning Amidoximate to Enhance Uranyl Binding: A Density Functional Theory Study
journal, October 2013
- Abney, Carter W.; Liu, Shubin; Lin, Wenbin
- The Journal of Physical Chemistry A, Vol. 117, Issue 45
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
Relativistic and correlation effects for element 105 (hahnium, Ha): a comparative study of M and MO (M = Nb, Ta, Ha) using energy-adjusted ab initio pseudopotentials
journal, June 1993
- Dolg, Michael; Stoll, Hermann; Preuss, Heinzwerner
- The Journal of Physical Chemistry, Vol. 97, Issue 22
Use of Solution-Phase Vibrational Frequencies in Continuum Models for the Free Energy of Solvation
journal, December 2011
- Ribeiro, Raphael F.; Marenich, Aleksandr V.; Cramer, Christopher J.
- The Journal of Physical Chemistry B, Vol. 115, Issue 49
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
Synthesis of Naphthalimidedioxime Ligand-Containing Fibers for Uranium Adsorption from Seawater
journal, December 2015
- Chatterjee, Sabornie; Bryantsev, Vyacheslav S.; Brown, Suree
- Industrial & Engineering Chemistry Research, Vol. 55, Issue 15
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
Complexation of glutarimidedioxime with Fe(iii), Cu(ii), Pb(ii), and Ni(ii), the competing ions for the sequestration of U(vi) from seawater
journal, January 2013
- Sun, Xiaoqi; Xu, Chao; Tian, Guoxin
- Dalton Transactions, Vol. 42, Issue 40
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
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
Theoretical study of the coordination behavior of formate and formamidoximate with dioxovanadium( v ) cation: implications for selectivity towards uranyl
journal, January 2015
- Mehio, Nada; Johnson, J. Casey; Dai, Sheng
- Physical Chemistry Chemical Physics, Vol. 17, Issue 47
Theoretical Study of Oxovanadium(IV) Complexation with Formamidoximate: Implications for the Design of Uranyl-Selective Adsorbents
journal, December 2015
- Mehio, Nada; Ivanov, Alexander S.; Ladshaw, Austin P.
- Industrial & Engineering Chemistry Research, Vol. 55, Issue 15
Computational Study of Copper(II) Complexation and Hydrolysis in Aqueous Solutions Using Mixed Cluster/Continuum Models
journal, August 2009
- Bryantsev, Vyacheslav S.; Diallo, Mamadou S.; Goddard, William A.
- The Journal of Physical Chemistry A, Vol. 113, Issue 34
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
Highly selective extraction of the uranyl ion with hydrophobic amidoxime-functionalized ionic liquids via η2 coordination
journal, January 2012
- Barber, Patrick S.; Kelley, Steven P.; Rogers, Robin D.
- RSC Advances, Vol. 2, Issue 22
Interaction of Metal Ions with Amidoximes 1a
journal, December 1959
- Pearse, George A.; Pflaum, Ronald T.
- Journal of the American Chemical Society, Vol. 81, Issue 24
Crystal structures of bis[2,2'-iminobis(acetamidoxime)]nickel(II) chloride dihydrate and bis[2,2'-iminobis(acetamidoxime)]copper(II) chloride
journal, August 1970
- Cullen, David L.; Lingafelter, Edward C.
- Inorganic Chemistry, Vol. 9, Issue 8
Bis(oxamide oxime)platinum(II) bis(perchlorate) dihydrate
journal, April 1982
- Endres, H.
- Acta Crystallographica Section B Structural Crystallography and Crystal Chemistry, Vol. 38, Issue 4
Stereochemistry of nucleic acids and their constituents. XXI. The crystal and molecular structure of bis-(4-aminoimidazole-5-carboxamidoxime)copper(II) perchlorate, a degradation product of adenine N 1 -oxide
journal, July 1972
- Stout, C. D.; Sundaralingam, M.; Lin, G. H. -Y.
- Acta Crystallographica Section B Structural Crystallography and Crystal Chemistry, Vol. 28, Issue 7
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
Alternative Alkaline Conditioning of Amidoxime Based Adsorbent for Uranium Extraction from Seawater
journal, October 2015
- Das, S.; Liao, W. -P.; Flicker Byers, M.
- Industrial & Engineering Chemistry Research, Vol. 55, Issue 15
The adsorption mechanism of uranium(VI) from seawater on a macroporous fibrous polymeric adsorbent containing amidoxime chelating functional group
journal, November 2003
- Zhang, Anyun; Asakura, Toshihide; Uchiyama, Gunzo
- Reactive and Functional Polymers, Vol. 57, Issue 1
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
Works referencing / citing this record:
Extraction and adsorption of U(VI) from aqueous solution using affinity ligand-based technologies: an overview
journal, July 2019
- Wang, Jianlong; Zhuang, Shuting
- Reviews in Environmental Science and Bio/Technology, Vol. 18, Issue 3
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
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
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