Enthalpy of formation of U3Si2: A high-temperature drop calorimetry study

Guo, Xiaofeng; White, Joshua T.; Nelson, Andrew T.; Migdisov, Artaches; Roback, Robert; Xu, Hongwu

doi:10.1016/j.jnucmat.2018.04.032

Title: Enthalpy of formation of U₃Si₂: A high-temperature drop calorimetry study

Abstract

U₃Si₂ is presently receiving consideration as a high density light water reactor fuel. A reliable knowledge of the formation enthalpy of U₃Si₂ not only helps study the thermal stability but also facilitate the modeling efforts by serving as a benchmark parameter for thermodynamic calculations of phase equilibria at high temperatures. Previous high temperature thermal analysis on U₃Si₂ laid the basis for us to conduct two types of high-temperature drop calorimetric measurements to determine its enthalpy of formation: oxide-melt drop-solution calorimetry and transposed temperature drop calorimetry, from which the results obtained are consistent. The determined standard enthalpy of formation of U₃Si₂ per mole atom, -33.2 ± 3.1 kJ/mol∙at.%, is in good agreement with previously reported values obtained by other techniques. Our drop calorimetry methods will be used for thermodynamic studies of other U-Si compounds whose enthalpies of formation are not available.

Authors:

^[1]; White, Joshua T. ^[2];

^[2]; Migdisov, Artaches ^[2]; Roback, Robert ^[2]; Xu, Hongwu ^[2]

Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Washington State Univ., Pullman, WA (United States). Dept. of Chemistry
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)

Publication Date:: Sat Apr 21 00:00:00 EDT 2018

Research Org.:: Los Alamos National Lab. (LANL), Los Alamos, NM (United States)

Sponsoring Org.:: USDOE Laboratory Directed Research and Development (LDRD) Program

OSTI Identifier:: 1479951

Alternate Identifier(s):: OSTI ID: 1532560

Report Number(s):: LA-UR-18-22051
Journal ID: ISSN 0022-3115

Grant/Contract Number:: AC52-06NA25396

Resource Type:: Accepted Manuscript

Journal Name:: Journal of Nuclear Materials

Additional Journal Information:: Journal Volume: 507; Journal Issue: C; Journal ID: ISSN 0022-3115

Publisher:: Elsevier

Country of Publication:: United States

Language:: English

Subject:: 36 MATERIALS SCIENCE; Uranium silicide; High temperature drop calorimetry; Enthalpy of formation

Citation Formats


                    Guo, Xiaofeng, White, Joshua T., Nelson, Andrew T., Migdisov, Artaches, Roback, Robert, and Xu, Hongwu. Enthalpy of formation of U3Si2: A high-temperature drop calorimetry study.  United States: N. p., 2018. 
Web.  doi:10.1016/j.jnucmat.2018.04.032.

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                    Guo, Xiaofeng, White, Joshua T., Nelson, Andrew T., Migdisov, Artaches, Roback, Robert, & Xu, Hongwu. Enthalpy of formation of U3Si2: A high-temperature drop calorimetry study.  United States.  https://doi.org/10.1016/j.jnucmat.2018.04.032

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                    Guo, Xiaofeng, White, Joshua T., Nelson, Andrew T., Migdisov, Artaches, Roback, Robert, and Xu, Hongwu. Sat .  
"Enthalpy of formation of U3Si2: A high-temperature drop calorimetry study".  United States.  https://doi.org/10.1016/j.jnucmat.2018.04.032.  https://www.osti.gov/servlets/purl/1479951.

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@article{osti_1479951,

  title        = {Enthalpy of formation of U3Si2: A high-temperature drop calorimetry study},

  author       = {Guo, Xiaofeng and White, Joshua T. and Nelson, Andrew T. and Migdisov, Artaches and Roback, Robert and Xu, Hongwu},

  abstractNote = {U3Si2 is presently receiving consideration as a high density light water reactor fuel. A reliable knowledge of the formation enthalpy of U3Si2 not only helps study the thermal stability but also facilitate the modeling efforts by serving as a benchmark parameter for thermodynamic calculations of phase equilibria at high temperatures. Previous high temperature thermal analysis on U3Si2 laid the basis for us to conduct two types of high-temperature drop calorimetric measurements to determine its enthalpy of formation: oxide-melt drop-solution calorimetry and transposed temperature drop calorimetry, from which the results obtained are consistent. The determined standard enthalpy of formation of U3Si2 per mole atom, -33.2 ± 3.1 kJ/mol∙at.%, is in good agreement with previously reported values obtained by other techniques. Our drop calorimetry methods will be used for thermodynamic studies of other U-Si compounds whose enthalpies of formation are not available.},

  doi          = {10.1016/j.jnucmat.2018.04.032},

  journal      = {Journal of Nuclear Materials},

  number       = C,

  volume       = 507,

  place        = {United States},

  year         = {Sat Apr 21 00:00:00 EDT 2018},

  month        = {Sat Apr 21 00:00:00 EDT 2018}

}

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Works referencing / citing this record:

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

Guo, Xiaofeng; Boukhalfa, Hakim; Mitchell, Jeremy N.
Review of Scientific Instruments, Vol. 90, Issue 4
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DOI: 10.1557/jmr.2019.192

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Title: Enthalpy of formation of U3Si2: A high-temperature drop calorimetry study

Abstract

Citation Formats

Thermophysical properties of U3Si to 1150K journal, September 2014

Thermophysical properties of U 3 Si 2 to 1773 K journal, September 2015

Thermophysical properties of U3Si5 to 1773 K journal, January 2015

Thermophysical properties of USi to 1673 K journal, April 2016

Oxidation behavior of U-Si compounds in air from 25 to 1000 C journal, February 2017

Non-stoichiometry in U3Si2 journal, December 2016

Amorphization of U3Si2 by ion or neutron irradiation journal, June 1996

Irradiation behaviour of uranium silicide compounds journal, February 2004

Accident tolerant fuels for LWRs: A perspective journal, May 2014

Short Communication on “In-situ TEM ion irradiation investigations on U3Si2 at LWR temperatures” journal, February 2017

Thermodynamic study of the U–Si system journal, May 2009

Phase equilibria in the U-Si system from first-principles calculations journal, October 2016

The effect of aluminum additions on the oxidation resistance of U3Si2 journal, June 2017

Crystal Structure and Thermodynamic Stability of Ba/Ti‐Substituted Pollucites for Radioactive Cs/Ba Immobilization journal, April 2015

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

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

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

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

Thermodynamic studies of studtite thermal decomposition pathways via amorphous intermediates UO3, U2O7, and UO4 journal, September 2016

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

Energetics of metastudtite and implications for nuclear waste alteration journal, November 2014

Thermochemistry of microporous silicotitanate phases in the Na 2 O–Cs 2 O–SiO 2 –TiO 2 –H 2 O system journal, March 2000

Energetics of Substituted Pollucites Along the CsAlSi 2 O 6 -CsTiSi 2 O 6.5 Join: A High-Temperature Calorimetric Study journal, March 2001

The Oxidation of Shaped Silicon Surfaces journal, June 1982

Oxidation property of silicon small particles journal, April 1991

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

Energetics of hydration on uranium oxide and peroxide surfaces journal, June 2019

Title: Enthalpy of formation of U₃Si₂: A high-temperature drop calorimetry study

Thermophysical properties of U3Si to 1150K
journal, September 2014

Thermophysical properties of $U_{3} {Si}_{2}$ to 1773 K
journal, September 2015

Thermophysical properties of U3Si5 to 1773 K
journal, January 2015

Thermophysical properties of USi to 1673 K
journal, April 2016

Oxidation behavior of U-Si compounds in air from 25 to 1000 C
journal, February 2017

Non-stoichiometry in U3Si2
journal, December 2016

Amorphization of U3Si2 by ion or neutron irradiation
journal, June 1996

Irradiation behaviour of uranium silicide compounds
journal, February 2004

Accident tolerant fuels for LWRs: A perspective
journal, May 2014

Short Communication on “In-situ TEM ion irradiation investigations on U3Si2 at LWR temperatures”
journal, February 2017

Thermodynamic study of the U–Si system
journal, May 2009

Phase equilibria in the U-Si system from first-principles calculations
journal, October 2016

The effect of aluminum additions on the oxidation resistance of U3Si2
journal, June 2017

Crystal Structure and Thermodynamic Stability of Ba/Ti‐Substituted Pollucites for Radioactive Cs/Ba Immobilization
journal, April 2015

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

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

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

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

Thermodynamic studies of studtite thermal decomposition pathways via amorphous intermediates UO3, U2O7, and UO4
journal, September 2016

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

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journal, March 2000

Energetics of Substituted Pollucites Along the CsAlSi ₂ O ₆ -CsTiSi ₂ O _6.5 Join: A High-Temperature Calorimetric Study
journal, March 2001

The Oxidation of Shaped Silicon Surfaces
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Oxidation property of silicon small particles
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Sample seal-and-drop device and methodology for high temperature oxide melt solution calorimetric measurements of PuO ₂
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