skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Uranium Dioxide in Ionic Liquid with a Tri-n-butylphosphate-HNO3 Complex - Dissolution and Coordination Environment

Journal Article · · Dalton Transactions
DOI:https://doi.org/10.1039/C0DT01518K· OSTI ID:1845876

Uranium dioxide can be dissolved directly in an imidiazolium-based ionic liquid (IL) at room temperature with a tri-n-butylphosphate(TBP)-HNO3 complex. The dissolution process follows pseudo first-order kinetics initially. Raman spectroscopic studies show the dissolved uranyl ions are coordinated with TBP in the IL phase with a molar ratio of (UO2)2+: TBP = 1:2. The dissolved uranyl species can be effectively transferred to supercritical fluid carbon dioxide (sc-CO2) phase. No aqueous phase is formed in either the IL dissolution or the supercritical fluid extraction process. Absorption spectra of the extracted uranyl species in the sc-CO2 phase suggests the presence of an UO2(TBP)2(NO3)2 and HNO3 adduct probably of the form UO2(TBP)2(NO3)2·HNO3. The adduct dissociates in a water-dodecane trap solution during pressure reduction resulting in UO2(TBP)2(NO3)2 collected in the dodecane phase.

Research Organization:
Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
Sponsoring Organization:
USDOE
DOE Contract Number:
AC05-76RL01830
OSTI ID:
1845876
Report Number(s):
PNNL-SA-78548
Journal Information:
Dalton Transactions, Vol. 40, Issue 18
Country of Publication:
United States
Language:
English

References (36)

Dissolution of UO2, UO3 and of some lanthanide oxides in BumimTf2N: effect of acid and water and formation of UO2(NO3)3– journal January 2007
Actinide and lanthanide speciation in imidazolium-based ionic liquids journal July 2009
Extraction of Uranium from Aqueous Solutions by Using Ionic Liquid and Supercritical Carbon Dioxide in Conjunction journal April 2009
Synergistic effects in the facilitated transfer of metal ions into room-temperature ionic liquids journal January 2005
A ternary mechanism for the facilitated transfer of metal ions into room-temperature ionic liquids (RTILs): implications for the “greenness” of RTILs as extraction solvents journal January 2005
Ionic Liquids as Extraction Solvents: Where do We Stand? journal June 2006
Anion concentration-dependent partitioning mechanism in the extraction of uranium into room-temperature ionic liquids journal April 2008
EXAFS Investigations of the Mechanism of Facilitated Ion Transfer into a Room-Temperature Ionic Liquid journal September 2002
Uranyl Coordination Environment in Hydrophobic Ionic Liquids:  An in Situ Investigation journal April 2003
Room-temperature ionic liquids: new solvents for f -element separations and associated solution chemistry journal February 2003
Identical extraction behavior and coordination of trivalent or hexavalent f-element cations using ionic liquid and molecular solvents journal January 2005
The coordination chemistry of actinides in ionic liquids: A review of experiment and simulation journal April 2006
Interactions of 1-Methylimidazole with UO 2 (CH 3 CO 2 ) 2 and UO 2 (NO 3 ) 2 :  Structural, Spectroscopic, and Theoretical Evidence for Imidazole Binding to the Uranyl Ion journal January 2007
Effect of Alkyl Group in 1-Alkyl-3-methylimidazolium Hexafluorophosphate Ionic Liquids on the Extraction of Uranium by Tri-n-butylphosphate Diluted with Ionic Liquids journal January 2004
Extraction of uranium(VI) from nitric acid medium by 1.1M tri-n-butylphosphate in ionic liquid diluent journal June 2005
Extraction of uranium (VI) by 1.1M tri-n-butylphosphate/ionic liquid and the feasibility of recovery by direct electrodeposition from organic phase journal January 2008
An investigation of the radiochemical stability of ionic liquids journal March 2002
Solvent extraction of strontium nitrate by a crown ether using room-temperature ionic liquids † journal January 1999
Formation of Higher Chloride Complexes of Np(IV) and Pu(IV) in Water-Stable Room-Temperature Ionic Liquid [BuMeIm][Tf 2 N] journal January 2006
Solvent extraction of U(vi) by task specific ionic liquids bearing phosphoryl groups journal January 2007
Novel class of functionalized ionic liquids with grafted CMPO-moieties for actinides and rare-earth elements recovery journal January 2010
The Radiation Chemistry of Ionic Liquids and its Implications for their Use in Nuclear Fuel Processing book December 2009
Lanthanides and Actinides in Ionic Liquids journal June 2007
Green processing using ionic liquids and CO2 journal May 1999
A Structural and Electrochemical Investigation of 1-Alkyl-3-methylimidazolium Salts of the Nitratodioxouranate(VI) Anions [{UO 2 (NO 3 ) 2 } 24 -C 2 O 4 )] 2- , [UO 2 (NO 3 ) 3 ] - , and [UO 2 (NO 3 ) 4 ] 2- journal April 2004
Characterization of Uranyl(VI) Nitrate Complexes in a Room Temperature Ionic Liquid Using Attenuated Total Reflection-Fourier Transform Infrared Spectrometry journal August 2010
Characterization of a Tri- n -butyl Phosphate−Nitric Acid Complex:  a CO 2 -Soluble Extractant for Dissolution of Uranium Dioxide journal October 2003
Kinetic study on dissolution of UO2 powders in nitric acid journal September 1995
Determination of Successive Complexation Constants in an Ionic Liquid: Complexation of UO 2 2+ with NO 3 in C 4 -mimTf 2 N Studied by UV−Vis Spectroscopy journal April 2010
Speciation of Uranyl Nitrato Complexes in Acetonitrile and in the Ionic Liquid 1-Butyl-3-methylimidazolium Bis(trifluoromethylsulfonyl)imide journal November 2007
Raman and Infrared Spectra and ab Initio Calculations of C 2 - 4 MIM Imidazolium Hexafluorophosphate Ionic Liquids journal September 2004
Raman spectroscopic studies of aqueous uranyl nitrate and perchlorate systems journal January 1980
Uranyl Coordination in Ionic Liquids:  The Competition between Ionic Liquid Anions, Uranyl Counterions, and Cl- Anions Investigated by Extended X-ray Absorption Fine Structure and UV−Visible Spectroscopies and Molecular Dynamics Simulations journal May 2007
Third Phase Formation Revisited: The U(VI), HNO 3 –TBP, n ‐Dodecane System journal January 2003
A high pressure fiber-optic reactor with charge-coupled device array ultraviolet-visible spectrometer for monitoring chemical processes in supercritical fluids journal December 1999
High solubility of UO2(NO3)2·2TBP complex in supercritical CO2 journal January 1998

Similar Records

Selective Extraction of Uranium from Liquid or Supercritical Carbon Dioxide
Technical Report · Tue Jul 31 00:00:00 EDT 2012 · OSTI ID:1845876

Extraction of Uranium from Aqueous Solutions Using Ionic Liquid and Supercritical Carbon Dioxide in Conjunction
Journal Article · Thu Jan 01 00:00:00 EST 2009 · Chemistry - A European Journal, 15(17):4458-4463 · OSTI ID:1845876

Supercritical Fluid Extraction of Radionuclides - A Green Technology for Nuclear Waste Management
Conference · Wed Sep 10 00:00:00 EDT 2003 · OSTI ID:1845876

Related Subjects