Applications of Alkali Metal Hydroxide Hydrofluxes to the Synthesis of Single-Crystal Ternary Actinide Oxides

Thomas, Evan L.; Stegman, Samantha; Skanthakumar, Suntharalingam; Wilson, Richard E.

doi:10.1002/chem.201904677

Title: Applications of Alkali Metal Hydroxide Hydrofluxes to the Synthesis of Single-Crystal Ternary Actinide Oxides

Abstract

Hydrofluxes are hydrated salts with melting points well below that of the dehydrated salt and boiling points well above that of water, affording a reaction medium, in which mild temperatures and pressures can be accessed for the synthesis of materials. Herein, the use of alkali metal hydroxide hydrofluxes for the synthesis of single crystal α-Na₂NpO₄ is described, and the single crystal X-ray structure of α-Na₂NpO₄, along with its X-ray absorption spectra and vibrational spectra, is reported. The ability to synthesize complex oxides of the actinides, in particular, transuranium materials, under mild conditions will serve to advance our ability to explore the structure–property relationships of the f elements.

Authors:

Thomas, Evan L. ^[1]; Stegman, Samantha ^[1]; Skanthakumar, Suntharalingam ^[1];

^[1]

Argonne National Lab. (ANL), Argonne, IL (United States)

Publication Date:: Thu Dec 05 00:00:00 EST 2019

Research Org.:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division

OSTI Identifier:: 1595677

Alternate Identifier(s):: OSTI ID: 1593177

Grant/Contract Number:: AC02-06CH11357

Resource Type:: Accepted Manuscript

Journal Name:: Chemistry - A European Journal

Additional Journal Information:: Journal Volume: 26; Journal Issue: 7; Journal ID: ISSN 0947-6539

Publisher:: ChemPubSoc Europe

Country of Publication:: United States

Language:: English

Subject:: 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; actinides; alkali metals; hydroxides; neptunium

Citation Formats


                    Thomas, Evan L., Stegman, Samantha, Skanthakumar, Suntharalingam, and Wilson, Richard E. Applications of Alkali Metal Hydroxide Hydrofluxes to the Synthesis of Single-Crystal Ternary Actinide Oxides.  United States: N. p., 2019. 
Web.  doi:10.1002/chem.201904677.

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                    Thomas, Evan L., Stegman, Samantha, Skanthakumar, Suntharalingam, & Wilson, Richard E. Applications of Alkali Metal Hydroxide Hydrofluxes to the Synthesis of Single-Crystal Ternary Actinide Oxides.  United States.  https://doi.org/10.1002/chem.201904677

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                    Thomas, Evan L., Stegman, Samantha, Skanthakumar, Suntharalingam, and Wilson, Richard E. Thu .  
"Applications of Alkali Metal Hydroxide Hydrofluxes to the Synthesis of Single-Crystal Ternary Actinide Oxides".  United States.  https://doi.org/10.1002/chem.201904677.  https://www.osti.gov/servlets/purl/1595677.

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@article{osti_1595677,

  title        = {Applications of Alkali Metal Hydroxide Hydrofluxes to the Synthesis of Single-Crystal Ternary Actinide Oxides},

  author       = {Thomas, Evan L. and Stegman, Samantha and Skanthakumar, Suntharalingam and Wilson, Richard E.},

  abstractNote = {Hydrofluxes are hydrated salts with melting points well below that of the dehydrated salt and boiling points well above that of water, affording a reaction medium, in which mild temperatures and pressures can be accessed for the synthesis of materials. Herein, the use of alkali metal hydroxide hydrofluxes for the synthesis of single crystal α-Na2NpO4 is described, and the single crystal X-ray structure of α-Na2NpO4, along with its X-ray absorption spectra and vibrational spectra, is reported. The ability to synthesize complex oxides of the actinides, in particular, transuranium materials, under mild conditions will serve to advance our ability to explore the structure–property relationships of the f elements.},

  doi          = {10.1002/chem.201904677},

  journal      = {Chemistry - A European Journal},

  number       = 7,

  volume       = 26,

  place        = {United States},

  year         = {Thu Dec 05 00:00:00 EST 2019},

  month        = {Thu Dec 05 00:00:00 EST 2019}

}

Copy to clipboard

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dataset (1)

Title: Applications of Alkali Metal Hydroxide Hydrofluxes to the Synthesis of Single-Crystal Ternary Actinide Oxides

Abstract

Citation Formats

Review of the Scientific Understanding of Radioactive Waste at the U.S. DOE Hanford Site journal, January 2018

Synthesis and crystal structure characterisation of sodium neptunate compounds journal, June 2011

Electrochemical and spectrophotometric investigations of neptunium in alkaline media journal, January 2001

Molten-Salt Reactor Chemistry journal, February 1970

Auf der Suche nach neuen Materialien: Kristallzucht von quaternären und höherwertigen Oxiden in Flussmitteln journal, January 2012

Crystal Growth of New Hexahydroxometallates Using a Hydroflux journal, September 2013

A short history of SHELX journal, December 2007

BESSRC-CAT bending magnet beamline at the advanced photon source journal, July 2001

Nuclear waste forms for actinides journal, March 1999

Cation−Cation Interactions and Antiferromagnetism in Na[Np(V)O 2 (OH) 2 ]: Synthesis, Structure, and Magnetic Properties journal, January 2007

α- and βNa2UO4: Structural and Thermochemical Relationships journal, March 1995

Hydroflux Crystal Growth of Platinum Group Metal Hydroxides: Sr 6 NaPd 2 (OH) 17 , Li 2 Pt(OH) 6 , Na 2 Pt(OH) 6 , Sr 2 Pt(OH) 8 , and Ba 2 Pt(OH) 8 journal, June 2012

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

Synthesis and structure of ditetrabutylammonium tetrachlorodioxoneptunium(VI) journal, November 2004

On the Mechanism of Oxygen Exchange Between Uranyl(VI) Oxygen and Water in Strongly Alkaline Solution as Studied by 17 O NMR Magnetization Transfer journal, June 2010

Hydroflux synthesis and crystal structure of new lanthanide tungstate oxyhydroxides journal, April 2015

Actinide structural studies. Part 1. Crystal and molecular structures of dinitratodioxobis(triphenylphosphine oxide)neptunium(VI), dinitratodioxobis(triphenylphosphine oxide)uranium(VI), and dichlorodioxo-(triphenylphosphine oxide)neptunium(VI) journal, January 1982

Synthesis and single crystal X-ray diffraction study of U(VI), Np(VI), and Pu(VI) perchlorate hydrates journal, August 2010

Vibrational spectra of alkali metal (Li, Na and K) uranates and consequent assignment of uranate ion site symmetry journal, July 1998

Uranium-oxygen lattice vibrations of lithium, β-sodium and β-strontium uranates journal, April 1970

Chemical Vapor Transport Reactions - A Historical Review journal, February 2013

Structural Properties and Charge Distribution of the Sodium Uranium, Neptunium, and Plutonium Ternary Oxides: A Combined X-ray Diffraction and XANES Study journal, February 2016

SIXPack a Graphical User Interface for XAS Analysis Using IFEFFIT journal, January 2005

Investigation of the UONa and (U,Pu)ONa phase diagrams — Study of Na3UO4 and Na3(U,Pu)O4 phases journal, November 1993

Molecular Hydroxo-Bridged Dimers of Uranium(VI), Neptunium(VI), and Plutonium(VI): [Me 4 N] 2 [(AnO 2 ) 2 (OH) 2 (NO 3 ) 4 ] journal, February 2019

Reactivity of the “yl”-Bond in Uranyl(VI) Complexes. 1. Rates and Mechanisms for the Exchange between the trans -dioxo Oxygen Atoms in (UO 2 ) 2 (OH) 2 2+ and Mononuclear UO 2 (OH) n 2- n Complexes with Solvent Water journal, October 2007

Mössbauer spectroscopy, magnetization, magnetic susceptibility, and low temperature heat capacity of α -Na 2 NpO 4 journal, January 2016

Materials Discovery by Flux Crystal Growth: Quaternary and Higher Order Oxides journal, January 2012

Uranium‐Oxygen Lattice Vibrations of α‐Sodium and Magnesium Monouranates journal, May 1972

Synthesis, structure, and optical properties of a series of quaternary oxides, K2Ba(MO4)2 (M = Cr, Mo, W) journal, February 2014

Chemical Speciation of Neptunium(VI) under Strongly Alkaline Conditions. Structure, Composition, and Oxo Ligand Exchange journal, June 2012

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Covalency in the actinide dioxides: Systematic study of the electronic properties using screened hybrid density functional theory journal, July 2007

Chemical Speciation of the Uranyl Ion under Highly Alkaline Conditions. Synthesis, Structures, and Oxo Ligand Exchange Dynamics journal, April 1999

Actinide structural studies. Part 2. Crystal and molecular structures of rubidium tris(nitrato)dioxoneptunate(1–) and sodium tris(acetato)dioxoneptunate(1–) journal, January 1982

Review of the Scientific Understanding of Radioactive Waste at the U.S. DOE Hanford Site
journal, January 2018

Synthesis and crystal structure characterisation of sodium neptunate compounds
journal, June 2011

Electrochemical and spectrophotometric investigations of neptunium in alkaline media
journal, January 2001

Molten-Salt Reactor Chemistry
journal, February 1970

Auf der Suche nach neuen Materialien: Kristallzucht von quaternären und höherwertigen Oxiden in Flussmitteln
journal, January 2012

Crystal Growth of New Hexahydroxometallates Using a Hydroflux
journal, September 2013

A short history of SHELX
journal, December 2007

BESSRC-CAT bending magnet beamline at the advanced photon source
journal, July 2001

Nuclear waste forms for actinides
journal, March 1999

Cation−Cation Interactions and Antiferromagnetism in Na[Np(V)O ₂ (OH) ₂ ]: Synthesis, Structure, and Magnetic Properties
journal, January 2007

α- and βNa2UO4: Structural and Thermochemical Relationships
journal, March 1995

Hydroflux Crystal Growth of Platinum Group Metal Hydroxides: Sr ₆ NaPd ₂ (OH) ₁₇ , Li ₂ Pt(OH) ₆ , Na ₂ Pt(OH) ₆ , Sr ₂ Pt(OH) ₈ , and Ba ₂ Pt(OH) ₈
journal, June 2012

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

Synthesis and structure of ditetrabutylammonium tetrachlorodioxoneptunium(VI)
journal, November 2004

On the Mechanism of Oxygen Exchange Between Uranyl(VI) Oxygen and Water in Strongly Alkaline Solution as Studied by ¹⁷ O NMR Magnetization Transfer
journal, June 2010

Hydroflux synthesis and crystal structure of new lanthanide tungstate oxyhydroxides
journal, April 2015

Actinide structural studies. Part 1. Crystal and molecular structures of dinitratodioxobis(triphenylphosphine oxide)neptunium(VI), dinitratodioxobis(triphenylphosphine oxide)uranium(VI), and dichlorodioxo-(triphenylphosphine oxide)neptunium(VI)
journal, January 1982

Synthesis and single crystal X-ray diffraction study of U(VI), Np(VI), and Pu(VI) perchlorate hydrates
journal, August 2010

Vibrational spectra of alkali metal (Li, Na and K) uranates and consequent assignment of uranate ion site symmetry
journal, July 1998

Uranium-oxygen lattice vibrations of lithium, β-sodium and β-strontium uranates
journal, April 1970

Chemical Vapor Transport Reactions - A Historical Review
journal, February 2013

Structural Properties and Charge Distribution of the Sodium Uranium, Neptunium, and Plutonium Ternary Oxides: A Combined X-ray Diffraction and XANES Study
journal, February 2016

SIXPack a Graphical User Interface for XAS Analysis Using IFEFFIT
journal, January 2005

Investigation of the UONa and (U,Pu)ONa phase diagrams — Study of Na3UO4 and Na3(U,Pu)O4 phases
journal, November 1993

Molecular Hydroxo-Bridged Dimers of Uranium(VI), Neptunium(VI), and Plutonium(VI): [Me 4 N] 2 [(AnO 2 ) 2 (OH) 2 (NO 3 ) 4 ]
journal, February 2019

Reactivity of the “yl”-Bond in Uranyl(VI) Complexes. 1. Rates and Mechanisms for the Exchange between the trans -dioxo Oxygen Atoms in (UO ₂ ) ₂ (OH) ₂ ²⁺ and Mononuclear UO ₂ (OH) _n ^2- ⁿ ^{Complexes with Solvent Water}
journal, October 2007

Mössbauer spectroscopy, magnetization, magnetic susceptibility, and low temperature heat capacity of α -Na 2 NpO 4
journal, January 2016

Materials Discovery by Flux Crystal Growth: Quaternary and Higher Order Oxides
journal, January 2012

Uranium‐Oxygen Lattice Vibrations of α‐Sodium and Magnesium Monouranates
journal, May 1972

Synthesis, structure, and optical properties of a series of quaternary oxides, K2Ba(MO4)2 (M = Cr, Mo, W)
journal, February 2014

Chemical Speciation of Neptunium(VI) under Strongly Alkaline Conditions. Structure, Composition, and Oxo Ligand Exchange
journal, June 2012

Synthesis, Structure, and Vibrational Properties of [Ph ₄ P] ₂ NpO ₂ Cl ₄ and [Ph ₄ P] ₂ PuO ₂ Cl ₄ Complexes
journal, March 2018

Covalency in the actinide dioxides: Systematic study of the electronic properties using screened hybrid density functional theory
journal, July 2007

Chemical Speciation of the Uranyl Ion under Highly Alkaline Conditions. Synthesis, Structures, and Oxo Ligand Exchange Dynamics
journal, April 1999

Actinide structural studies. Part 2. Crystal and molecular structures of rubidium tris(nitrato)dioxoneptunate(1–) and sodium tris(acetato)dioxoneptunate(1–)
journal, January 1982