Thermodynamics of CeSiO4: Implications for Actinide Orthosilicates

Strzelecki, Andrew; Bourgeois, Clement; Kriegsman, Kyle; Estevenon, Paul; Wei, Nian; Szenknect, Stephanie; Mesbah, Adel; Wu, Di; Ewing, Rodney C.; Dacheux, Nicolas; Guo, Xiaofeng

doi:10.1021/acs.inorgchem.0c01476

Title: Thermodynamics of CeSiO₄: Implications for Actinide Orthosilicates

Abstract

Zircon (ZrSiO₄: I4₁/amd) can accommodate actinides, such as thorium, uranium, and plutonium. The zircon structure has been determined for several of the end member compositions of other actinides, such as plutonium and neptunium. However, the thermodynamic properties of these actinide zircon structure-types are largely unknown due to the difficulties in synthesizing these materials and handling transuranium actinides. Thus, we have completed a thermodynamic study of cerium orthosilicate, stetindite (CeSiO₄), a surrogate of PuSiO₄. For the first time, the standard enthalpy of formation of CeSiO₄ was obtained by high temperature oxide melt solution calorimetry to be -1971.9 ± 3.6 kJ/mol. Stetindite is energetically metastable with respect to CeO₂ and SiO₂ by 27.5 ± 3.1 kJ/mol. The metastability explains the rarity of the natural occurrence of stetindite and the difficulty of its synthesis. Applying the obtained enthalpy of formation of CeSiO₄ from this work, along with those previously reported for USiO₄ and ThSiO₄, we developed an empirical energetic relation for actinide orthosilicates. Here, the predicted enthalpies of formation of AnSiO₄ are then made with a discussion of future strategies to efficiently immobilize Pu or minor actinides in the zircon structure.

Authors:

Strzelecki, Andrew ^[1]; Bourgeois, Clement ^[1]; Kriegsman, Kyle ^[1]; Estevenon, Paul ^[2]; Wei, Nian ^[3]; Szenknect, Stephanie ^[4]; Mesbah, Adel ^[4]; Wu, Di ^[1]; Ewing, Rodney C. ^[5]; Dacheux, Nicolas ^[4];

^[1]

Washington State University, Pullman, WA (United States)
Univ. Montpellier, Bagnols sur Ceze (France); Univ. Montpellier, Marcoule (France)
Washington State University, Pullman, WA (United States); Sichuan University, Chengdu (China)
Univ. Montpellier, Bagnols sur Ceze (France)
Stanford Univ., CA (United States)

Publication Date:: 2020-09-01

Research Org.:: Washington State Univ., Pullman, WA (United States)

Sponsoring Org.:: USDOE Office of Nuclear Energy (NE)

OSTI Identifier:: 1651197

Grant/Contract Number:: NE0008582

Resource Type:: Accepted Manuscript

Journal Name:: Inorganic Chemistry

Additional Journal Information:: Journal Volume: 59; Journal Issue: 18; Journal ID: ISSN 0020-1669

Publisher:: American Chemical Society (ACS)

Country of Publication:: United States

Language:: English

Subject:: 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Cerium orthosilicate; thermodynamics; enthalpy of formation; ceramic waste forms; rare earth minerals; actinide geochemistry; lanthanide geochemistry; stetindite

Citation Formats


                    Strzelecki, Andrew, Bourgeois, Clement, Kriegsman, Kyle, Estevenon, Paul, Wei, Nian, Szenknect, Stephanie, Mesbah, Adel, Wu, Di, Ewing, Rodney C., Dacheux, Nicolas, and Guo, Xiaofeng. Thermodynamics of CeSiO4: Implications for Actinide Orthosilicates.  United States: N. p., 2020. 
Web.  doi:10.1021/acs.inorgchem.0c01476.

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                    Strzelecki, Andrew, Bourgeois, Clement, Kriegsman, Kyle, Estevenon, Paul, Wei, Nian, Szenknect, Stephanie, Mesbah, Adel, Wu, Di, Ewing, Rodney C., Dacheux, Nicolas, & Guo, Xiaofeng. Thermodynamics of CeSiO4: Implications for Actinide Orthosilicates.  United States.  https://doi.org/10.1021/acs.inorgchem.0c01476

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                    Strzelecki, Andrew, Bourgeois, Clement, Kriegsman, Kyle, Estevenon, Paul, Wei, Nian, Szenknect, Stephanie, Mesbah, Adel, Wu, Di, Ewing, Rodney C., Dacheux, Nicolas, and Guo, Xiaofeng. Tue .  
"Thermodynamics of CeSiO4: Implications for Actinide Orthosilicates".  United States.  https://doi.org/10.1021/acs.inorgchem.0c01476.  https://www.osti.gov/servlets/purl/1651197.

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@article{osti_1651197,

  title        = {Thermodynamics of CeSiO4: Implications for Actinide Orthosilicates},

  author       = {Strzelecki, Andrew and Bourgeois, Clement and Kriegsman, Kyle and Estevenon, Paul and Wei, Nian and Szenknect, Stephanie and Mesbah, Adel and Wu, Di and Ewing, Rodney C. and Dacheux, Nicolas and Guo, Xiaofeng},

  abstractNote = {Zircon (ZrSiO4: I41/amd) can accommodate actinides, such as thorium, uranium, and plutonium. The zircon structure has been determined for several of the end member compositions of other actinides, such as plutonium and neptunium. However, the thermodynamic properties of these actinide zircon structure-types are largely unknown due to the difficulties in synthesizing these materials and handling transuranium actinides. Thus, we have completed a thermodynamic study of cerium orthosilicate, stetindite (CeSiO4), a surrogate of PuSiO4. For the first time, the standard enthalpy of formation of CeSiO4 was obtained by high temperature oxide melt solution calorimetry to be -1971.9 ± 3.6 kJ/mol. Stetindite is energetically metastable with respect to CeO2 and SiO2 by 27.5 ± 3.1 kJ/mol. The metastability explains the rarity of the natural occurrence of stetindite and the difficulty of its synthesis. Applying the obtained enthalpy of formation of CeSiO4 from this work, along with those previously reported for USiO4 and ThSiO4, we developed an empirical energetic relation for actinide orthosilicates. Here, the predicted enthalpies of formation of AnSiO4 are then made with a discussion of future strategies to efficiently immobilize Pu or minor actinides in the zircon structure.},

  doi          = {10.1021/acs.inorgchem.0c01476},

  journal      = {Inorganic Chemistry},

  number       = 18,

  volume       = 59,

  place        = {United States},

  year         = {2020},

  month        = {9}

}

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Title: Thermodynamics of CeSiO4: Implications for Actinide Orthosilicates

Abstract

Citation Formats

Multiparametric Study of the Synthesis of ThSiO 4 under Hydrothermal Conditions journal, July 2018

Groundwater Nanoparticles in the Far-Field at the Nevada Test Site: Mechanism for Radionuclide Transport journal, March 2009

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Cerium Substitution in Yttrium Iron Garnet: Valence State, Structure, and Energetics journal, December 2013

TiO 2 Stability Landscape: Polymorphism, Surface Energy, and Bound Water Energetics journal, December 2006

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The Transuranium Elements journal, October 1946

Diamylamylphosphonate Solvent Extraction of Am(VI) from Nuclear Fuel Raffinate Simulant Solution journal, August 2012

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How To Explain the Difficulties in the Coffinite Synthesis from the Study of Uranothorite? journal, November 2011

Structure and thermodynamics of uranium-containing iron garnets journal, September 2016

FIRST OBSERVATION OF AQUEOUS TETRAVALENT CURIUM 1 journal, September 1961

A linear free energy relationship for crystalline solids and aqueous ions journal, March 1992

Radiation-induced defects and amorphization in zircon journal, November 1990

The incorporation of hydroxyl groups and molecular water in natural zircon (ZrSiO4) journal, December 2001

Feasibility Limits in Using Cerium as a Surrogate for Plutonium Incorporation in Zircon, Zirconia and Pyrochlore journal, January 2000

Calorimetric study of molten sodium molybdate-molybdenum trioxide mixtures at 970.degree.K journal, November 1967

Synthesis of Coffinite, USiO 4 , and Structural Investigations of U x Th (1– x ) SiO 4 Solid Solutions journal, December 2013

Enthalpies of formation of U-, Th-, Ce-brannerite: implications for plutonium immobilization journal, August 2003

Structure and Chemistry of Zircon and Zircon-Group Minerals journal, January 2003

Thermodynamic properties of soddyite from solubility and calorimetry measurements journal, April 2007

Performance Assessment of Zircon as a Waste Form for Excess Weapons Plutonium Under Deep Borehole Burial Conditions journal, January 1995

The Design and Evaluation of Nuclear-Waste Forms: Clues from Mineralogy journal, June 2001

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Enthalpies of formation of rare earth orthovanadates, REVO4 journal, March 2007

The Gibbs free energies and enthalpies of formation of U (super 6+) phases; an empirical method of prediction journal, April 1999

Formation enthalpies of LaLn׳O3 (Ln׳=Ho, Er, Tm and Yb) interlanthanide perovskites journal, July 2015

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Thermal Expansion of Compounds of Zircon Structure journal, May 1990

Displaced by radiation journal, January 2007

Colloid Transport of Plutonium in the Far-Field of the Mayak Production Association, Russia journal, October 2006

Kinetics of antigorite dehydration: A real-time X-ray diffraction study journal, August 2005

Radiation effects in crystalline ceramics for the immobilization of high-level nuclear waste and plutonium journal, June 1998

Formation enthalpy of ThSiO4 and enthalpy of the thorite → huttonite phase transition journal, October 2005

Alpha-Decay-Induced Amorphization in Complex Silicate Structures journal, July 1993

Sample seal-and-drop device and methodology for high temperature oxide melt solution calorimetric measurements of PuO 2 journal, April 2019

Americium and curium journal, January 1959

Contemporary Chemistry of Berkelium and Californium journal, June 2019

Uranium transport in acidic brines under reducing conditions journal, April 2018

Title: Thermodynamics of CeSiO₄: Implications for Actinide Orthosilicates

Multiparametric Study of the Synthesis of ThSiO ₄ under Hydrothermal Conditions
journal, July 2018

Groundwater Nanoparticles in the Far-Field at the Nevada Test Site: Mechanism for Radionuclide Transport
journal, March 2009

Quantification of actinide α-radiation damage in minerals and ceramics
journal, January 2007

Long-term storage of spent nuclear fuel
journal, February 2015

Thermochemistry of rare-earth orthophosphates
journal, September 2001

Lanthanide and Actinide Chemistry
book, January 2006

Laboratory investigation of the role of desorption kinetics on americium transport associated with bentonite colloids
journal, October 2015

Revised effective ionic radii and systematic studies of interatomic distances in halides and chalcogenides
journal, September 1976

Use of linear free energy relationship to predict Gibbs free energies of formation of pyrochlore phases (CaMTi2O7)
journal, November 1999

Cerium Substitution in Yttrium Iron Garnet: Valence State, Structure, and Energetics
journal, December 2013

TiO ₂ Stability Landscape: Polymorphism, Surface Energy, and Bound Water Energetics
journal, December 2006

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journal, January 2020

Implications of the thermal properties and kinetic parameters of dehydroxylation of mica minerals for fault weakening, frictional heating, and earthquake energetics
journal, July 2011

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journal, January 2005

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journal, August 1952

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journal, June 2019

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journal, March 2005

The Transuranium Elements
journal, October 1946

Diamylamylphosphonate Solvent Extraction of Am(VI) from Nuclear Fuel Raffinate Simulant Solution
journal, August 2012

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journal, February 2010

Zircon: A host-phase for the disposal of weapons plutonium
journal, February 1995

Thermodynamic and structural evolution of mechanically milled and swift heavy ion irradiated Er2Ti2O7 pyrochlore
journal, December 2019

Investigation of Pu Incorporation into Zircon Single Crystal
journal, January 2004

Formation of CeSiO ₄ from cerium( iii ) silicate precursors
journal, January 2019

How To Explain the Difficulties in the Coffinite Synthesis from the Study of Uranothorite?
journal, November 2011

Structure and thermodynamics of uranium-containing iron garnets
journal, September 2016

FIRST OBSERVATION OF AQUEOUS TETRAVALENT CURIUM ¹
journal, September 1961

A linear free energy relationship for crystalline solids and aqueous ions
journal, March 1992

Radiation-induced defects and amorphization in zircon
journal, November 1990

The incorporation of hydroxyl groups and molecular water in natural zircon (ZrSiO4)
journal, December 2001

Feasibility Limits in Using Cerium as a Surrogate for Plutonium Incorporation in Zircon, Zirconia and Pyrochlore
journal, January 2000

Calorimetric study of molten sodium molybdate-molybdenum trioxide mixtures at 970.degree.K
journal, November 1967

Synthesis of Coffinite, USiO ₄ , and Structural Investigations of U _x Th _{(1– x )} SiO ₄ Solid Solutions
journal, December 2013

Enthalpies of formation of U-, Th-, Ce-brannerite: implications for plutonium immobilization
journal, August 2003

Structure and Chemistry of Zircon and Zircon-Group Minerals
journal, January 2003

Thermodynamic properties of soddyite from solubility and calorimetry measurements
journal, April 2007

Performance Assessment of Zircon as a Waste Form for Excess Weapons Plutonium Under Deep Borehole Burial Conditions
journal, January 1995

The Design and Evaluation of Nuclear-Waste Forms: Clues from Mineralogy
journal, June 2001

High-Uranium Zircon from "Chernobyl Lavas"
journal, January 1993

Enthalpies of formation of rare earth orthovanadates, REVO4
journal, March 2007

The Gibbs free energies and enthalpies of formation of U (super 6+) phases; an empirical method of prediction
journal, April 1999

Formation enthalpies of LaLn׳O3 (Ln׳=Ho, Er, Tm and Yb) interlanthanide perovskites
journal, July 2015

U( v ) in metal uranates: a combined experimental and theoretical study of MgUO ₄ , CrUO ₄ , and FeUO ₄
journal, January 2016

Thermochemistry of La1−xLnxPO4-monazites (Ln= Gd, Eu)
journal, February 2017

Enthalpies of formation of polyhalite: A mineral relevant to salt repository
journal, November 2017

Effects of bentonite heating on U(VI) adsorption
journal, October 2019

The new mineral stetindite, CeSiO<SUB>4</SUB>, a cerium end-member of the zircon group
journal, August 2009

First experimental determination of the solubility constant of coffinite
journal, May 2016

Coffinitization - A Mechanism for the Alteration of UO ₂ under Reducing Conditions
journal, January 1991

Enthalpies of formation of Ce-pyrochlore, Ca0.93Ce1.00Ti2.035O7.00, U-pyrochlore, Ca1.46U4+0.23U6+0.46Ti1.85O7.00 and Gd-pyrochlore, Gd2Ti2O7: three materials relevant to the proposed waste form for excess weapons plutonium
journal, June 2002

Soft Hydrothermal Synthesis of Hafnon, HfSiO ₄
journal, January 2020

Nuclear Fuel in a Reactor Accident
journal, March 2012

Hydrothermal Synthesis of Advanced Ceramic Powders
journal, October 2006

Radiation effects in nuclear waste forms for high-level radioactive waste
journal, January 1995

Hydrothermal stability studies of the zircon-thorite group
journal, January 1961

From thorite to coffinite: A spectroscopic study of Th1−xUxSiO4 solid solutions
journal, January 2014

Preparation of CeSiO ₄ from aqueous precursors under soft hydrothermal conditions
journal, January 2019

Energetics of a Uranothorite (Th _{1– x} U _x SiO ₄ ) Solid Solution
journal, September 2016

Amorphous Alumina Nanoparticles: Structure, Surface Energy, and Thermodynamic Phase Stability
journal, August 2013

Phase Diagrams for Ceramists: Supplement no. 1
journal, December 1949

Application of a linear free energy relationship to crystalline solids of MO2 and M(OH)4
journal, August 1999

Thermodynamics of formation of coffinite, USiO ₄
journal, May 2015

Synthesis of nuclear waste monazites, ideal actinide hosts for geologic disposal
journal, November 1978

Coffinite, USiO ₄ , Is Abundant in Nature: So Why Is It So Difficult To Synthesize?
journal, July 2015

Optical study and analysis of ${Pu}^{4 +}$ in single crystals of ${ZrSiO}_{4}$
journal, April 1989

Direct measurements of water adsorption enthalpy on hafnia and zirconia
journal, October 2005

Thermal Expansion of Compounds of Zircon Structure
journal, May 1990

Displaced by radiation
journal, January 2007

Colloid Transport of Plutonium in the Far-Field of the Mayak Production Association, Russia
journal, October 2006

Kinetics of antigorite dehydration: A real-time X-ray diffraction study
journal, August 2005

Radiation effects in crystalline ceramics for the immobilization of high-level nuclear waste and plutonium
journal, June 1998

Formation enthalpy of ThSiO4 and enthalpy of the thorite → huttonite phase transition
journal, October 2005

Alpha-Decay-Induced Amorphization in Complex Silicate Structures
journal, July 1993

Sample seal-and-drop device and methodology for high temperature oxide melt solution calorimetric measurements of PuO ₂
journal, April 2019

Americium and curium
journal, January 1959

Contemporary Chemistry of Berkelium and Californium
journal, June 2019

Uranium transport in acidic brines under reducing conditions
journal, April 2018

Impact of Carbonate Ions on the Synthesis of ThSiO ₄ under Hydrothermal Conditions
journal, September 2018

Evaluation of f-element borate chemistry
journal, September 2016