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Title: Detection and identification of solids, surfaces, and solutions of uranium using vibrational spectroscopy

Journal Article · · Coordination Chemistry Reviews
 [1];  [2];  [2]
  1. Univ. of Iowa, Iowa City, IA (United States); University of Iowa
  2. Univ. of Iowa, Iowa City, IA (United States)

The purpose of this review is to provide an overview of uranium speciation using vibrational spectroscopy methods including Raman and IR. Uranium is a naturally occurring, radioactive element that is utilized in the nuclear energy and national security sectors. Fundamental uranium chemistry is also an active area of investigation due to ongoing questions regarding the participation of 5f orbitals in bonding, variation in oxidation states and coordination environments, and unique chemical and physical properties. Importantly, uranium speciation affects fate and transportation in the environment, influences bioavailability and toxicity to human health, controls separation processes for nuclear waste, and impacts isotopic partitioning and geochronological dating. This work provides a thorough discussion of the vibrational modes for U(IV), U(V), and U(VI) and applications of infrared absorption and Raman scattering spectroscopies in the identification and detection of both naturally occurring and synthetic uranium species in solid and solution states. The vibrational frequencies of the uranyl moiety, including both symmetric and asymmetric stretches are sensitive to the coordinating ligands and used to identify individual species in water, organic solvents, and ionic liquids or on the surface of materials. Additionally, vibrational spectroscopy allows for the in situ detection and real-time monitoring of chemical reactions involving uranium. Finally, techniques to enhance uranium species signals with vibrational modes are discussed to expand the application of vibrational spectroscopy to biological, environmental, inorganic, and materials scientists and engineers.

Research Organization:
Univ. of Iowa, Iowa City, IA (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division
Grant/Contract Number:
SC0013980
OSTI ID:
1668719
Alternate ID(s):
OSTI ID: 1612053
Journal Information:
Coordination Chemistry Reviews, Journal Name: Coordination Chemistry Reviews Vol. 374; ISSN 0010-8545
Publisher:
ElsevierCopyright Statement
Country of Publication:
United States
Language:
English

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Resonance Raman excitation profile for uranyl acetate in dimethyl sulfoxide journal July 1999
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One-dimensional uranium(VI) coordination polymers with pyridinecarboxylate ligands journal July 2016
Raman spectroscopic determination of formation constant of uranyl hydrolysis species (UO2)2(OH)22+ journal July 2001
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Tetrameric entity resulting from two distinct dinuclear uranyl-centered motifs bridged through μ2-OH and pyridazine-3,6-dicarboxylate journal February 2011
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How to Bend the Uranyl Cation via Crystal Engineering journal February 2018
Coordination Trends in Alkali Metal Crown Ether Uranyl Halide Complexes:  The Series [A(Crown)] 2 [UO 2 X 4 ] Where A = Li, Na, K and X = Cl, Br journal July 2001
The resonance Raman effect of dicaesium uranyl tetrachloride in dimethyl sulfoxide journal August 2001
Raman and infrared spectroscopic studies of the uranyl ion: the symmetric stretching frequency, force constants, and bond lengths journal January 1969
Near- and mid-infrared spectroscopy of the uranyl selenite mineral haynesite (UO2)3(SeO3)2(OH)2·5H2O journal January 2009
The structure of uranyl chloride monohydrate by neutron diffraction and the disorder of the water molecule journal January 1974
The Formula of Uranyl Ion journal July 1949
Pentavalent uranium chemistry—synthetic pursuit of a rare oxidation state journal January 2009
Uranium(VI) hybrid materials with [(UO 2 ) 33 -O)(µ 2 -OH) 3 ] + as the sub-building unit via uranyl-cation interactions journal January 2016
Structural Polarity Induced by Cooperative Hydrogen Bonding and Lone-Pair Alignment in the Molecular Uranyl Iodate Na 2 [UO 2 (IO 3 ) 4 (H 2 O)] journal October 2006
Identification of the +2 Oxidation State for Uranium in a Crystalline Molecular Complex, [K(2.2.2-Cryptand)][(C 5 H 4 SiMe 3 ) 3 U] journal August 2013
Chemical controls on uranyl citrate speciation and the self-assembly of nanoscale macrocycles and sandwich complexes in aqueous solutions journal January 2015
A structural study on uranyl (VI) nitrate complexes with cyclic amides: N-n-butyl-2-pyrrolidone, N-cyclohexylmethyl-2-pyrrolidone, and 1,3-dimethyl-2-imidazolidone journal March 2005
Probing the Nature of Chemical Bonding in Uranyl(VI) Complexes with Quantum Chemical Methods journal November 2012
Effect of Amorphous Fe(III) Oxide Transformation on the Fe(II)-Mediated Reduction of U(VI) journal February 2011
Mica Surfaces Stabilize Pentavalent Uranium journal May 2005
Structural and Vibrational Properties of U(VI)O 2 Cl 4 2- and Pu(VI)O 2 Cl 4 2- Complexes journal November 2013
Impact of Natural Organic Matter on Uranium Transport through Saturated Geologic Materials: From Molecular to Column Scale journal May 2012
Impact of the uranium (VI) speciation in mineralised urines on its extraction by calix[6]arene bearing hydroxamic groups used in chromatography columns journal November 2015
The reaction of water on polycrystalline UO2: Pathways to surface and bulk oxidation journal June 2005
Excitation profile of the resonance Raman effect of rubidium uranyl trinitrate in dimethyl sulfoxide journal April 1997
Spectroscopy and DFT studies of uranyl carbonate, rutherfordine, UO 2 CO 3 : a model for uranium transport, carbon dioxide sequestration, and seawater species journal November 2017
Incorporation of Oxidized Uranium into Fe (Hydr)oxides during Fe(II) Catalyzed Remineralization journal October 2009
The crystal structure of synthetic autunite, Ca[(UO 2 )(PO 4 )] 2 (H 2 O) 11 journal January 2003
Thermodynamics of U(VI) and Eu(III) complexation by unsaturated carboxylates journal May 2011
Raman studies of the vibrational dynamics and phase transitions in uranyl nitrate hexahydrate journal May 1989
Raman spectroscopic study of the uranyl carbonate mineral čejkaite and its comparison with synthetic trigonal Na 4 [UO 2 (CO 3 ) 3 ]: Raman spectroscopic study of čejkaite journal May 2009
Shumwayite, [(UO 2 )(SO 4 )(H 2 O) 2 ] 2 ·H 2 O, a new uranyl sulfate mineral from Red Canyon, San Juan County, Utah, USA journal April 2017
Crystal Structures and Synthesis of the Copper-Dominant Members of the Autunite and Meta-Autunite Groups: Torbernite, Zeunerite, Metatorbernite and Metazeunerite journal April 2003
Spent Nuclear Fuel journal December 2006
Raman spectroscopic study of the uranyl phosphate mineral dewindtite journal January 2006
Uranium speciation in waters of different uranium mining areas journal June 1998
The effect of thermodynamic data on computer model predictions of uranium speciation in natural water systems journal June 2002
New NMR evidence on the uranylcitrate complexes journal June 1987
Synthesis of a Uranyl Persulfide Complex and Quantum Chemical Studies of Formation and Topologies of Hypothetical Uranyl Persulfide Cage Clusters journal April 2012
A Raman spectroscopic study of the uranyl sulphate mineral johannite journal September 2005
Actinide Carbonte Complexes and Their Importance in Actinide Environmental Chemistry journal January 1995
Neutron powder profile studies of the gamma uranium trioxide phases journal January 1977
Investigations of Crystal-Chemical Variability in lead Uranyl Oxide Hydrates. i. Curite journal June 2000
Structural Versatility of Uranyl(VI) Nitrate Complexes That Involve the Diamide Ligand Et2N(C=O)(CH2)n(C=O)NEt2 (0 ≤ n ≤ 6) journal July 2012
Upscaling Sorption/Desorption Processes in Reactive Transport Models To Describe Metal/Radionuclide Transport: A Critical Review journal November 2010
The nature of ammonium uranates journal June 1973
Luminescence spectrum of Cs2UO2Cl4 journal January 1978
Engaging the Terminal: Promoting Halogen Bonding Interactions with Uranyl Oxo Atoms journal August 2017
Syntheses and spectroscopic characterization of uranium(VI) silicate minerals journal October 2007
Spectral Analysis of the Uranyl Squarate and Croconate System: Evaluating Differences between the Solution and Solid-State Phases journal September 2017
Nuclear applications of inorganic mass spectrometry: NUCLEAR APPLICATIONS OF INORGANIC MS journal October 2009
Two Systems of [DabcoH 2 ] 2+ /[PipH 2 ] 2+ –Uranyl–Oxalate Showing Reversible Crystal-to-Crystal Transformations Controlled by the Diammonium/Uranyl/Oxalate Ratios in Aqueous Solutions ([DabcoH 2 ] 2+ = 1,4-Diazabicyclo-[2.2.2]-octaneH 2 and [PipH 2 ] 2+ = PiperazineH 2 ) journal April 2013
Uranium determination using atomic spectrometric techniques: An overview journal August 2010
Micro-Raman Spectrum of Triuranium Octoxide, U 3 O 8 journal July 1988
Influence of extreme conditions on the formation and structures of caesium uranium( vi ) arsenates journal January 2015
Crystal structure and formula revision of deliensite, Fe[(UO 2 ) 2 (SO 4 ) 2 (OH) 2 ](H 2 O) 7 journal December 2012
Raman spectroscopic study of the uranyl selenite mineral demesmaekerite Pb 2 Cu 5 (UO 2 ) 2 (SeO 3 ) 6 (OH) 6 ·2H 2 O journal May 2009
Crystal structure of the uranyl-oxide mineral rameauite [Crystal structure of the uranyl-oxide mineral rameauite] journal January 2016
Sulfate-Centered Sodium-Icosahedron-Templated Uranyl Peroxide Phosphate Cages with Uranyl Bridged by μ–η 12 Peroxide journal January 2017
Vibrational spectroscopic studies of uranyl complexes in aqueous and non-aqueous solutions journal January 1992
Excitation Profile of the Resonance Raman Effect of Uranyl Nitrate in Dimethyl Sulfoxide journal February 1995
Understanding the origins of O yl –U–O yl bending in the uranyl (UO 2 2+ ) ion journal January 2018
Structurally Characterized Ternary U−O−N Compound, UN 4 O 12 :  UO 2 (NO 3 ) 2 ·N 2 O 4 or NO + UO 2 (NO 3 ) 3 - ? journal November 2005
K 3 (U 3 O 6 )(Si 2 O 7 ) and Rb 3 (U 3 O 6 )(Ge 2 O 7 ): A Pentavalent-Uranium Silicate and Germanate journal June 2008
Binary and ternary uranium(vi) humate complexes studied by attenuated total reflection Fourier-transform infrared spectroscopy journal January 2011
Chemical Speciation of the Uranyl Ion under Highly Alkaline Conditions. Synthesis, Structures, and Oxo Ligand Exchange Dynamics journal April 1999
Investigating Actinyl Oxo Cations by X-ray Absorption Spectroscopy journal November 2003
Utilizing bifurcated halogen-bonding interactions with the uranyl oxo group in the assembly of a UO 2 –3-bromo-5-iodobenzoic acid coordination polymer journal March 2017
Spectroscopic studies on the uranyl-schiff base solid complex (N,N'-p-phenylenebis(salicylideneiminato)UO2) journal January 1992
Binary and ternary surface complexes of U(VI) on the gibbsite/water interface studied by vibrational and EXAFS spectroscopy journal October 2012
Coordination structures for uranyl carboxylate complexes in aqueous solution studied by IR and carbon-13 NMR spectra journal November 1987
Vibrational spectroscopy of synthetic analogues of ankoleite, chernikovite and intermediate solid solution journal March 2016
Study of the alteration products of a natural uraninite by Raman spectroscopy journal July 2015
Mid-, far-infrared and raman spectra of uranyl complexes in aqueous solutions journal January 1984
Physical Characterization and Reactivity of the Uranyl Peroxide [UO 22 -O 2 )(H 2 O) 2 ]·2H 2 O: Implications for Storage of Spent Nuclear Fuels journal July 2012
Raman spectroscopy of uranopilite of different origins—implications for molecular structure journal January 2007
Corrosion of uranium dioxide in hydrogen peroxide solutions journal May 2004
The Structure of Uranyl Sulfate in Aqueous Solution — Monodentate Versus Bidentate Coordination
  • Hennig, C.; Schmeide, K.; Brendler, V.
  • X-RAY ABSORPTION FINE STRUCTURE - XAFS13: 13th International Conference, AIP Conference Proceedings https://doi.org/10.1063/1.2644495
conference January 2007
Evaluation of the Behavior of Uranium Peroxocarbonate Complexes in Na–U(VI)–CO 3 –OH–H 2 O 2 Solutions by Raman Spectroscopy journal November 2012
Raman spectroscopic study of the uranyl tellurite mineral moctezumite PbUO 2 (TeO 3 ) 2 journal January 2009
Raman spectroscopic studies of defect structures and phase transition in hyper-stoichiometric UO2+x journal January 2010
Self-Assembly of Uranyl-Peroxide Nanocapsules in Basic Peroxidic Environments journal May 2016
Aqueous uranium complexes. 2. Raman spectroscopic study of the complex formation of the dioxouranium(VI) ion with a variety of inorganic and organic ligands journal December 1992
The complexation of uranium(VI) and atmospherically derived CO2 at the ferrihydrite–water interface probed by time-resolved vibrational spectroscopy journal July 2012
Expanding the Remarkable Structural Diversity of Uranyl Tellurites:  Hydrothermal Preparation and Structures of K[UO 2 Te 2 O 5 (OH)], Tl 3 {(UO 2 ) 2 [Te 2 O 5 (OH)](Te 2 O 6 )}·2H 2 O, β-Tl 2 [UO 2 (TeO 3 ) 2 ], and Sr 3 [UO 2 (TeO 3 ) 2 ](TeO 3 ) 2 journal October 2002
Uranium( vi ) complexes with isonicotinic acid: from monomer to 2D polymer with unique U–N bonding journal January 2015
Infrared and Raman spectroscopic study of uranyl complexes: hydroxide and acetate derivatives in aqueous solution journal November 1998
Raman spectroscopic study of the uranyl selenite mineral marthozite Cu[(UO 2 ) 3 (SeO 3 ) 2 O 2 ]·8H 2 O: Raman spectroscopic study of Cu[(UO 2 ) 3 (SeO 3 ) 2 O 2 ]·8H 2 O journal May 2008
Density Functional Theory Study of the Complexation of the Uranyl Dication with Anionic Phosphate Ligands with and without Water Molecules journal September 2013
Raman and Infrared Spectral Studies of Aqueous Calcium Nitrate Solutions journal January 1967
U6+ Minerals and Inorganic Compounds: Insights into an Expanded Structural Hierarchy of Crystal Structures journal December 2005
Infrared and raman spectra (solid state) of uranyl 2,4-pentanedionate: UO2(acac)2 journal March 1995
Raman spectroscopic study of the uranyl phosphate mineral dumontite Pb 2 [(UO 2 ) 3 O 2 (PO 4 ) 2 ]·5H 2 O journal June 2009
Crystal chemical studies of the 5 f -series of elements. XXIII. On the crystal chemistry of uranyl compounds and of related compounds of transuranic elements journal December 1954
Raman spectroscopic study of the uranyl carbonate mineral zellerite journal January 2008
Molecular structure of the uranyl silicates—a Raman spectroscopic study journal January 2006
Vibrational spectroscopic study of hydrated uranyl oxide: Curite journal August 2007
A Raman spectroscopic study of the uranyl carbonate rutherfordine journal January 2007
Structural characterization of environmentally relevant ternary uranyl citrate complexes present in aqueous solutions and solid state materials journal January 2015
METARAUCHITE, Ni(UO2)2(AsO4)2{middle dot}8H2O, FROM JACHYMOV, CZECH REPUBLIC, AND SCHNEEBERG, GERMANY: A NEW MEMBER OF THE AUTUNITE GROUP journal April 2010
XAFS investigation of polyamidoxime-bound uranyl contests the paradigm from small molecule studies journal January 2016
A Raman spectroscopic study of uranyl minerals from Cornwall, UK journal January 2014
The structural and spectroscopic characterisation of three actinyl complexes with coordinated and uncoordinated perrhenate: [UO 2 (ReO 4 ) 2 (TPPO) 3 ], [{(UO 2 )(TPPO) 3 } 22 -O 2 )][ReO 4 ] 2 and [NpO 2 (TPPO) 4 ][ReO 4 ] journal January 2004
Structural and spectroscopic characterization of two new layered uranyl(VI) p-xylenediphosphonate compounds synthesized via ionothermal method journal August 2015
Occurence of an Octanuclear Motif of Uranyl Isophthalate with Cation–Cation Interactions through Edge-Sharing Connection Mode journal July 2011
Optical properties of tetravalent uranium complexes in non-aqueous media journal September 2014
Raman Spectroscopic and ESI-MS Characterization of Uranyl Peroxide Cage Clusters journal January 2014
Raman spectroscopic study of the uranyl mineral, compreignacite, K 2 [(UO 2 ) 3 O 2 (OH) 3 ] 2 ·7H 2 O journal September 2008
Fourier transform infrared and Raman spectra of uranyl bis(2-hydroxybenzaldehyde): UO2(sal)2 journal November 2000
Uranium Mill Tailings: Geochemistry, Mineralogy, and Environmental Impact journal December 2006
Vibrational spectroscopy of selected natural uranyl vanadates journal October 2005
Uranyl complexes with the pyridine-2,6-dicarboxylato ligand: new dinuclear species with μ-η2,η2-peroxide, μ2-hydroxide or μ2-methoxide bridges journal January 2005
Uranyl (1,3-diphenylpropane-1,3-dionato) complexes with N-adamantylacetamide and azacyclononanone: Synthesis, spectroscopy, luminescence and crystal structures journal August 2006
Raman spectroscopic study of the uranyl sulphate mineral jáchymovite (UO 2 ) 8 (SO 4 )(OH) 14 · 13H 2 O: RS study of the mineral jáchymovite journal February 2009
Sorption of radionuclides from aqueous systems onto graphene oxide-based materials: a review journal January 2015
Influence of Dynamical Conditions on the Reduction of U VI at the Magnetite−Solution Interface journal January 2010
Uranyl peroxide clusters stabilized by dicarboxylate ligands: A pentagonal ring and a dimer with extensive uranyl–cation interactions journal May 2015
An X-ray crystallographic, Raman, and infrared spectral study of crystalline potassium uranyl carbonate, K 4 UO 2 (CO 3 ) 3 journal August 1980
Vorlanite (CaU6+)O4--A new mineral from the Upper Chegem caldera, Kabardino-Balkaria, Northern Caucasus, Russia journal December 2010
Tris-amidoximate uranyl complexes via η 2 binding mode coordinated in aqueous solution shown by X-ray absorption spectroscopy and density functional theory methods journal February 2018
The Propensity of Uranium-Peroxide Systems to Preserve Nanosized Assemblies journal July 2017
New ligands for uranium complexation: A stable uranyl dimer bearing 2,6-diacetylpyridine dioxime journal April 2017
Charge-Assisted Hydrogen-Bonding and Crystallization Effects within U VI Glycine Compounds : Charge-Assisted Hydrogen-Bonding and Crystallization Effects within U journal April 2017
Observation of the Surface-Enhanced Raman Scattering Spectrum of Uranyl Ion journal April 1996
Raman spectroscopy of walpurgite journal January 2006
Recent advances in computational actinoid chemistry journal January 2012
Density functional theory investigations on the binding modes of amidoximes with uranyl ions journal January 2016
Evaluating Best Practices in Raman Spectral Analysis for Uranium Speciation and Relative Abundance in Aqueous Solutions journal December 2015
Spectroscopy of UO 2 Cl 4 2 - in Basic Aluminum Chloride−1-Ethyl-3-methylimidazolium Chloride journal April 2001
The Crystal Structure of Na 6 [(UO 2 )(SO 4 ) 4 ](H 2 O) 4 : X-Ray and Raman Spectroscopy Study journal August 2015
Bioreduction of Uranium:  Environmental Implications of a Pentavalent Intermediate journal August 2005
Exploring Actinide Materials Through Synchrotron Radiation Techniques journal August 2014
Stoichiometries and Thermodynamic Stabilities for Aqueous Sulfate Complexes of U(VI) journal March 2008

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In Situ Generation of Organic Peroxide to Create a Nanotubular Uranyl Peroxide Phosphate journal November 2019
Interaction of An VI with Isothiocyanate Ion in Water-Organic Media (An = U, Np, Pu) : Interaction of An journal November 2019
Ionic liquids with polychloride anions as effective oxidants for the dissolution of UO 2 journal January 2019
Actinyl-cation interactions: experimental and theoretical assessment of [Np( vi )O 2 Cl 4 ] 2− and [U( vi )O 2 Cl 4 ] 2− systems journal January 2019
In Situ Generation of Organic Peroxide to Create a Nanotubular Uranyl Peroxide Phosphate journal November 2019
Layer-structured uranyl-oxide hydroxy-hydrates with Pr( iii ) and Tb( iii ) ions: hydroxyl to oxo transition driven by interlayer cations journal January 2020
Formation of a uranyl hydroxide hydrate via hydration of [(UO 2 F 2 )(H 2 O)] 7 ·4H 2 O journal January 2019
Two New Coordination Polymers with UO 2 2+ Units and Fluorinated Aromatic Carboxylate Linkers journal January 2020
Combined experimental and first-principles studies of a hydrated uranyl carbonate: Insight into phonon spectra for a core environmental class of uranium materials journal March 2020
Mineralogy, Crystallography and Structural Complexity of Natural Uranyl Silicates journal November 2018
Impacts of hydrogen bonding interactions with Np( v / vi )O 2 Cl 4 complexes: vibrational spectroscopy, redox behavior, and computational analysis journal January 2020