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

Abstract

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 involvingmore » 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.« less

Authors:
 [1];  [1];  [1]
  1. Univ. of Iowa, Iowa City, IA (United States)
Publication Date:
Research Org.:
Univ. of Iowa, Iowa City, IA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division
OSTI Identifier:
1668719
Grant/Contract Number:  
SC0013980
Resource Type:
Accepted Manuscript
Journal Name:
Coordination Chemistry Reviews
Additional Journal Information:
Journal Volume: 374; Journal ID: ISSN 0010-8545
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEAR CHEMISTRY; uranium; Raman; vibrational spectroscopy; infrared

Citation Formats

Lu, Grace, Haes, Amanda J., and Forbes, Tori Z. Detection and identification of solids, surfaces, and solutions of uranium using vibrational spectroscopy. United States: N. p., 2018. Web. doi:10.1016/j.ccr.2018.07.010.
Lu, Grace, Haes, Amanda J., & Forbes, Tori Z. Detection and identification of solids, surfaces, and solutions of uranium using vibrational spectroscopy. United States. https://doi.org/10.1016/j.ccr.2018.07.010
Lu, Grace, Haes, Amanda J., and Forbes, Tori Z. Tue . "Detection and identification of solids, surfaces, and solutions of uranium using vibrational spectroscopy". United States. https://doi.org/10.1016/j.ccr.2018.07.010. https://www.osti.gov/servlets/purl/1668719.
@article{osti_1668719,
title = {Detection and identification of solids, surfaces, and solutions of uranium using vibrational spectroscopy},
author = {Lu, Grace and Haes, Amanda J. and Forbes, Tori Z.},
abstractNote = {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.},
doi = {10.1016/j.ccr.2018.07.010},
journal = {Coordination Chemistry Reviews},
number = ,
volume = 374,
place = {United States},
year = {Tue Jul 31 00:00:00 EDT 2018},
month = {Tue Jul 31 00:00:00 EDT 2018}
}

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Computationally-Guided Assignment of Unexpected Signals in the Raman Spectra of Uranyl Triperoxide Complexes
journal, January 2017


Series of Uranyl-4,4′-biphenyldicarboxylates and an Occurrence of a Cation–Cation Interaction: Hydrothermal Synthesis and in Situ Raman Studies
journal, July 2013

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Raman spectroscopy of uranopilite of different origins—implications for molecular structure
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Near- and mid-infrared spectroscopy of the uranyl selenite mineral haynesite (UO2)3(SeO3)2(OH)2·5H2O
journal, January 2009

  • Frost, Ray L.; Čejka, Jiří
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A Raman and infrared spectroscopic study of the uranyl silicates—Weeksite, soddyite and haiweeite: Part 2
journal, February 2006

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Raman spectra of uranyl fluoro and thiocyanato complexes
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Laser raman spectroscopy of some uranyl trinitrate complexes (MUO2(NO3)3; M = Cs, Rb, K, NH4)
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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

  • Frost, Ray L.; Čejka, Jiří; Dickfos, Marilla J.
  • Journal of Raman Spectroscopy, Vol. 40, Issue 5
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Solubility properties of synthetic and natural meta-torbernite
journal, November 2013


[H 2 bipy] 2 [(UO 2 ) 6 Zn 2 (PO 3 OH) 4 (PO 4 ) 4 ]·H 2 O: An Open-Framework Uranyl Zinc Phosphate Templated by Diprotonated 4,4′-Bipyridyl
journal, October 2008

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Raman spectroscopic study of the uranyl oxyhydroxide hydrates: becquerelite, billietite, curite, schoepite and vandendriesscheite
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  • Frost, Ray L.; Čejka, Jiří; Weier, Matt L.
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Uranium Mill Tailings: Geochemistry, Mineralogy, and Environmental Impact
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Infrared and raman spectra (solid state) of uranyl 2,4-pentanedionate: UO2(acac)2
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Silver-Doped Sol−Gel Film as a Surface-Enhanced Raman Scattering Substrate for Detection of Uranyl and Neptunyl Ions
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Raman studies of the vibrational dynamics and phase transitions in uranyl nitrate hexahydrate
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A Raman spectroscopic study of the uranyl phosphate mineral threadgoldite
journal, November 2006

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U6+ Minerals and Inorganic Compounds: Insights into an Expanded Structural Hierarchy of Crystal Structures
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The influence of precipitation conditions on the properties of ammonium diuranate and uranium dioxide powders
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Exploring Optical and Vibrational Properties of the Uranium Carbonate Andersonite with Spectroscopy and First-Principles Calculations
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Role of uranium speciation in the uptake and translocation of uranium by plants
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Cation–cation interactions and cation exchange in a series of isostructural framework uranyl tungstates
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Crystal structure of UO2SO4·2.5H2O: Full anisotropic refinement and vibration characteristics
journal, November 2009


Raman spectra of stoichiometric and hyperstoichiometric uranium dioxide
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Study of uranyl sorption onto hematite by in situ attenuated total reflection–infrared spectroscopy
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Stoichiometry and Structure of Uranyl(VI) Hydroxo Dimer and Trimer Complexes in Aqueous Solution
journal, December 2007

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Molecular structure of the uranyl mineral uranopilite—a Raman spectroscopic study
journal, January 2005


Interaction between aqueous uranium (VI) and sulfide minerals: Spectroscopic evidence for sorption and reduction
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Raman spectroscopic study of the uranyl carbonate mineral zellerite
journal, January 2008

  • Frost, Ray L.; Dickfos, Marilla J.; Čejka, Jiří
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A Raman spectroscopic study of the uranyl phosphate mineral parsonsite
journal, January 2006

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Sorption of radionuclides from aqueous systems onto graphene oxide-based materials: a review
journal, January 2015

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Actinide Carbonte Complexes and Their Importance in Actinide Environmental Chemistry
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Intercalation of Iodic Acid into the Layered Uranyl Iodate, UO 2 (IO 3 ) 2 (H 2 O)
journal, January 2007

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A Trigonal Bipyramidal Uranyl Amido Complex:  Synthesis and Structural Characterization of [Na(THF) 2 ][UO 2 (N(SiMe 3 ) 2 ) 3 ]
journal, November 2000

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Probing the Nature of Chemical Bonding in Uranyl(VI) Complexes with Quantum Chemical Methods
journal, November 2012

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Porous Uranyl Borophosphates with Unique Three-Dimensional Open-Framework Structures
journal, July 2017


A Raman spectroscopic study of the uranyl selenite mineral haynesite
journal, January 2006

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Infrared spectra of some uranyl nitrate complexes
journal, September 1967


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

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Synthesis and characterization of 1:1 layered uranyl silicate mineral phases
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Upscaling Sorption/Desorption Processes in Reactive Transport Models To Describe Metal/Radionuclide Transport: A Critical Review
journal, November 2010

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Uranyl Peroxide Nanocluster (U 60 ) Persistence and Sorption in the Presence of Hematite
journal, February 2018

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Crystal structure of bassetite and saléeite: new insight into autunite-group minerals [Crystal structure of bassetite and saléeite: new insight into autunite-group minerals]
journal, September 2016

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A Raman spectroscopic study of the uranyl mineral rutherfordine-revisited
journal, September 2009

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New ligands for uranium complexation: A stable uranyl dimer bearing 2,6-diacetylpyridine dioxime
journal, April 2017

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Structural and Vibrational Properties of U(VI)O 2 Cl 4 2- and Pu(VI)O 2 Cl 4 2- Complexes
journal, November 2013

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Raman spectroscopic and SEM analysis of sodium-zippeite
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Sorption of uranium (VI) species on zircon: structural investigation of the solid/solution interface
journal, May 2003


The structure of uranyl chloride monohydrate by neutron diffraction and the disorder of the water molecule
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Uranium speciation in waters of different uranium mining areas
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Understanding the origins of O yl –U–O yl bending in the uranyl (UO 2 2+ ) ion
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SERS detection of uranyl using functionalized gold nanostars promoted by nanoparticle shape and size
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Mineral–Water Interface Reactions of Actinides
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XAFS investigation of polyamidoxime-bound uranyl contests the paradigm from small molecule studies
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Uranium speciation in biofilms studied by laser fluorescence techniques
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Effect of Amorphous Fe(III) Oxide Transformation on the Fe(II)-Mediated Reduction of U(VI)
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The resonance Raman effect of dicaesium uranyl tetrachloride in dimethyl sulfoxide
journal, August 2001


Sequestering ability of polycarboxylic ligands towards dioxouranium(VI)
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Fourier transform infrared and Raman spectra of uranyl bis(2-hydroxybenzaldehyde): UO2(sal)2
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Investigating Actinyl Oxo Cations by X-ray Absorption Spectroscopy
journal, November 2003

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Crystallization in Ionic Liquids: Synthesis, Properties, and Polymorphs of Uranyl Salts
journal, October 2014

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Synthesis and Structure of the [(UO 2 )S 4 ] 6– Anion: A Cation-Stabilized Uranyl Sulfide
journal, September 2013

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Raman spectroscopic study of the uranyl tricarbonate mineral liebigite
journal, March 2005


Probing the Influence of N-Donor Capping Ligands on Supramolecular Assembly in Molecular Uranyl Materials
journal, December 2015

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The effect of thermodynamic data on computer model predictions of uranium speciation in natural water systems
journal, June 2002

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A Raman spectroscopic study of the uranyl sulphate mineral johannite
journal, September 2005

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On the “yl” bond weakening in uranyl(VI) coordination complexes
journal, January 2011


Lattice Solvent and Crystal Phase Effects on the Vibrational Spectra of UO 2 Cl 4 2–
journal, September 2014

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Binary and ternary uranium(vi) humate complexes studied by attenuated total reflection Fourier-transform infrared spectroscopy
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Raman spectroscopic study of the uranyl mineral pseudojohannite Cu6.5[(UO2)4O4(SO4)2]2(OH)5·25H2O
journal, December 2009

  • Frost, Ray L.; Plášil, Jakub; Čejka, Jiří
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Aqueous Uranium(VI) Hydrolysis Species Characterized by Attenuated Total Reflection Fourier-Transform Infrared Spectroscopy
journal, November 2008

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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

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How to Bend the Uranyl Cation via Crystal Engineering
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Solution and Solid-State Structural Chemistry of Actinide Hydrates and Their Hydrolysis and Condensation Products
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Adsorption of Uranium over NH 2 -Functionalized Ordered Silica in Aqueous Solutions
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Assessing hand-held Raman spectrometer FirstDefender RM for nuclear safeguards applications
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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


Closing Uranyl Polyoxometalate Capsules with Bismuth and Lead Polyoxocations
journal, September 2016

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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

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Oxidizing dissolution mechanism of an irradiated MOX fuel in underwater aerated conditions at slightly acidic pH
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Pentavalent uranium chemistry—synthetic pursuit of a rare oxidation state
journal, January 2009

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Studtite, [(UO 2 )(O 2 )(H 2 O) 2 ](H 2 O) 2 : The first structure of a peroxide mineral
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Influence of extreme conditions on the formation and structures of caesium uranium( vi ) arsenates
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Solution coordination chemistry of actinides: Thermodynamics, structure and reaction mechanisms
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Electrochemical Behavior of U(VI) in Imidazolium Ionic Liquid Medium Containing Tri-n-butyl Phosphate and Chloride Ion and Spectroscopic Characterization of Uranyl Species
journal, September 2017

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Uranium-bearing phases in Hanford nuclear waste
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A Raman spectroscopic study of the uranyl tellurite mineral schmitterite
journal, November 2006

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Synthesis and characterization of francoisite-(Nd): Nd[(UO2)3O(OH)(PO4)2]{middle dot}6H2O
journal, February 2011

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Occurence of an Octanuclear Motif of Uranyl Isophthalate with Cation–Cation Interactions through Edge-Sharing Connection Mode
journal, July 2011

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A detailed study of UO2 to U3O8 oxidation phases and the associated rate-limiting steps
journal, September 2006


Synthesis and Structural Characterization of Hydrolysis Products within the Uranyl Iminodiacetate and Malate Systems
journal, August 2013

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Luminescence spectrum of Cs2UO2Cl4
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Copper(I) and Copper(II) Uranyl Heterometallic Hybrid Materials
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Density Functional Theory Study of the Complexation of the Uranyl Dication with Anionic Phosphate Ligands with and without Water Molecules
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Silver Nanoparticle Decorated Reduced Graphene Oxide (rGO) Nanosheet: A Platform for SERS Based Low-Level Detection of Uranyl Ion
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Raman spectroscopic study of the uranyl phosphate minerals phosphuranylite and yingjiangite
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Actinide speciation using X-ray absorption fine structure spectroscopy
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Spectroscopic Confirmation of Uranium(VI)−Carbonato Adsorption Complexes on Hematite
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Investigations of Crystal-Chemical Variability in lead Uranyl Oxide Hydrates. i. Curite
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Hydrolysis of Uranyl(VI) in Acidic and Basic Aqueous Solutions Using a Noncomplexing Organic Base: A Multivariate Spectroscopic and Statistical Study
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Speciation Studies of Metals in Trace Concentrations: The Mononuclear Uranyl(VI) Hydroxo Complexes
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Uranyl-Peroxide Clusters Incorporating Iron Trimers and Bridging by Bisphosphonate- and Carboxylate-Containing Ligands
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Ab Initio Investigation of the UO 3 Polymorphs: Structural Properties and Thermodynamic Stability
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Raman and Infrared Spectral Studies of Aqueous Calcium Nitrate Solutions
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Evaluating Best Practices in Raman Spectral Analysis for Uranium Speciation and Relative Abundance in Aqueous Solutions
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Vorlanite (CaU6+)O4--A new mineral from the Upper Chegem caldera, Kabardino-Balkaria, Northern Caucasus, Russia
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The complexation of uranium(VI) and atmospherically derived CO2 at the ferrihydrite–water interface probed by time-resolved vibrational spectroscopy
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Coordination structures for uranyl carboxylate complexes in aqueous solution studied by IR and carbon-13 NMR spectra
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Raman spectroscopy of uranyl rare earth carbonate kamotoite-(Y)
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Infrared and Raman spectra of uranyl(VI) oxo-hydroxo complexes in acid aqueous solutions: a chemometric study
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Synchrotron X-ray fluorescence microprobe: A microanalytical instrument for trace element studies in geochemistry, cosmochemistry, and the soil and environmental sciences
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Optical spectroscopic studies of the sorption of UO2+2 species on a reference smectite
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Works referencing / citing this record:

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  • Dalton Transactions, Vol. 48, Issue 36
  • DOI: 10.1039/c9dt02835h

Layer-structured uranyl-oxide hydroxy-hydrates with Pr( iii ) and Tb( iii ) ions: hydroxyl to oxo transition driven by interlayer cations
journal, January 2020

  • Lu, Kimbal Thane; Zhang, Yingjie; Wei, Tao
  • Dalton Transactions, Vol. 49, Issue 18
  • DOI: 10.1039/d0dt00526f

Interaction of An VI with Isothiocyanate Ion in Water-Organic Media (An = U, Np, Pu) : Interaction of An
journal, November 2019

  • Fedoseev, Aleksander; Charushnikova, Iraida; Budantseva, Nina
  • Zeitschrift für anorganische und allgemeine Chemie, Vol. 645, Issue 22
  • DOI: 10.1002/zaac.201900243

Mineralogy, Crystallography and Structural Complexity of Natural Uranyl Silicates
journal, November 2018