Fabrication and thermophysical property characterization of UN/U3Si2 composite fuel forms

White, Joshua Taylor; Travis, Austin William; Dunwoody, John Tyler; Nelson, Andrew Thomas

doi:10.1016/j.jnucmat.2017.08.041

Title: Fabrication and thermophysical property characterization of UN/U₃Si₂ composite fuel forms

Abstract

High uranium density composite fuels composed of UN and U₃Si₂ have been fabricated using a liquid phase sintering route at temperatures between 1873 K and 1973 K and spanning compositions of 10 vol% to 40 vol% U₃Si₂. Microstructural analysis and phase characterization revealed the formation of an U-Si-N phase of unknown structure. Microcracking was observed in the U-Si portion of the composite microstructure that likely originates from the mismatched coefficient of thermal expansion between the UN and U₃Si₂ leading to stresses on heating and cooling of the composite. Thermal expansion coefficient, thermal diffusivity, and thermal conductivity were characterized for each of the compositions as a function of temperature to 1673 K. Hysteresis is observed in the thermal diffusivity for the 20 vol% through 40 vol% specimens between room temperature and 1273 K, which is attributed to the microcracking in the U-Si phase. Thermal conductivity of the composites was modeled using the MOOSE framework based on the collected microstructure data. In conclusion, the impact of irradiation on thermal conductivity was also simulated for this class of composite materials.

Authors:

White, Joshua Taylor ^[1]; Travis, Austin William ^[2]; Dunwoody, John Tyler ^[1];

^[1]

Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Univ. of California, Irvine, CA (United States)

Publication Date:: 2017-09-21

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

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

OSTI Identifier:: 1414134

Alternate Identifier(s):: OSTI ID: 1549217

Report Number(s):: LA-UR-17-20508
Journal ID: ISSN 0022-3115; TRN: US1800659

Grant/Contract Number:: AC52-06NA25396; NE0000711

Resource Type:: Accepted Manuscript

Journal Name:: Journal of Nuclear Materials

Additional Journal Information:: Journal Volume: 495; Journal Issue: C; Journal ID: ISSN 0022-3115

Publisher:: Elsevier

Country of Publication:: United States

Language:: English

Subject:: 11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS; Material Science; Accident tolerant fuels; Composite nuclear fuel; Uranium mononitride; Uranium silicide

Citation Formats


                    White, Joshua Taylor, Travis, Austin William, Dunwoody, John Tyler, and Nelson, Andrew Thomas. Fabrication and thermophysical property characterization of UN/U3Si2 composite fuel forms.  United States: N. p., 2017. 
Web.  doi:10.1016/j.jnucmat.2017.08.041.

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                    White, Joshua Taylor, Travis, Austin William, Dunwoody, John Tyler, & Nelson, Andrew Thomas. Fabrication and thermophysical property characterization of UN/U3Si2 composite fuel forms.  United States.  https://doi.org/10.1016/j.jnucmat.2017.08.041

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                    White, Joshua Taylor, Travis, Austin William, Dunwoody, John Tyler, and Nelson, Andrew Thomas. Thu .  
"Fabrication and thermophysical property characterization of UN/U3Si2 composite fuel forms".  United States.  https://doi.org/10.1016/j.jnucmat.2017.08.041.  https://www.osti.gov/servlets/purl/1414134.

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@article{osti_1414134,

  title        = {Fabrication and thermophysical property characterization of UN/U3Si2 composite fuel forms},

  author       = {White, Joshua Taylor and Travis, Austin William and Dunwoody, John Tyler and Nelson, Andrew Thomas},

  abstractNote = {High uranium density composite fuels composed of UN and U3Si2 have been fabricated using a liquid phase sintering route at temperatures between 1873 K and 1973 K and spanning compositions of 10 vol% to 40 vol% U3Si2. Microstructural analysis and phase characterization revealed the formation of an U-Si-N phase of unknown structure. Microcracking was observed in the U-Si portion of the composite microstructure that likely originates from the mismatched coefficient of thermal expansion between the UN and U3Si2 leading to stresses on heating and cooling of the composite. Thermal expansion coefficient, thermal diffusivity, and thermal conductivity were characterized for each of the compositions as a function of temperature to 1673 K. Hysteresis is observed in the thermal diffusivity for the 20 vol% through 40 vol% specimens between room temperature and 1273 K, which is attributed to the microcracking in the U-Si phase. Thermal conductivity of the composites was modeled using the MOOSE framework based on the collected microstructure data. In conclusion, the impact of irradiation on thermal conductivity was also simulated for this class of composite materials.},

  doi          = {10.1016/j.jnucmat.2017.08.041},

  journal      = {Journal of Nuclear Materials},

  number       = C,

  volume       = 495,

  place        = {United States},

  year         = {2017},

  month        = {9}

}

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Works referencing / citing this record:

Uranium nitride-silicide advanced nuclear fuel: higher efficiency and greater safety
journal, October 2018

Wilson, Tashiema L.; Moore, Emily E.; Adorno Lopes, Denise
Advances in Applied Ceramics, Vol. 117, Issue sup1
DOI: 10.1080/17436753.2018.1521607

A first-principles study on the influences of metal species Al, Zr, Mo and Tc on the mechanical properties of U ₃ Si ₂
journal, January 2020

Gao, Haigen; Liu, Yande; Hu, Jun
Physical Chemistry Chemical Physics, Vol. 22, Issue 4
DOI: 10.1039/c9cp03814k

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Title: Fabrication and thermophysical property characterization of UN/U3Si2 composite fuel forms

Abstract

Citation Formats

Formation of uranium mononitride by the reaction of uranium dioxide with carbon in ammonia and a mixture of hydrogen and nitrogen— I synthesis of high purity UN journal, December 1977

Investigation of the reaction UO2+x + PuO2 + C + N2 by thermogravimetry journal, August 1988

Preparation of uranium nitride in the form of microspheres journal, June 1992

The sintering of uranium mononitride journal, October 1965

Sintering of UN as a Function of Temperature and N2 Pressure journal, July 1971

Kinetics of the oxidation of UN and U(CO) in carbon dioxide, steam and water at elevated temperatures journal, January 1966

Oxidation of uranium mononitride and uranium monocarbide journal, January 1966

Hydrolysis of uranium mononitride journal, January 1967

Oxidation of uranium mononitride journal, September 1975

Oxidation and hydrolysis kinetic studies on UN journal, November 1991

Dual phase MgO–ZrO2 ceramics for use in LWR inert matrix fuel journal, June 2005

Neutronic performance of uranium nitride composite fuels in a PWR journal, August 2014

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

Uranium silicide pellet fabrication by powder metallurgy for accident tolerant fuel evaluation and irradiation journal, November 2015

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

Degradation of UN and UN–U 3 Si 2 pellets in steam environment journal, January 2017

Development of an accident-tolerant fuel composite from uranium mononitride (UN) and uranium sesquisilicide (U3 Si2) with increased uranium loading journal, April 2016

Fabrication and microstructural analysis of UN-U3Si2 composites for accident tolerant fuel applications journal, August 2016

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

A new high-pressure phase of uranium nitride studied by X-ray diffraction and synchrotron radiation journal, February 1985

Structural chemistry and magnetic behavior of binary uranium silicides journal, April 1992

NIH Image to ImageJ: 25 years of image analysis journal, June 2012

Improvement of the mathematical modeling of flash measurements journal, January 2002

Flash Method of Determining Thermal Diffusivity, Heat Capacity, and Thermal Conductivity journal, September 1961

Material property correlations for uranium mononitride journal, May 1990

Thermophysical properties of U3Si5 to 1773 K journal, January 2015

Material property correlations for uranium mononitride journal, May 1990

Material property correlations for uranium mononitride journal, May 1990

Evaluation of Rule-of-Mixtures Predictions of Thermal Expansion in Powder-Processed Ni-Al2O3 Composites journal, October 1999

Theory of thermal expansion of composites journal, March 1988

OOF: an image-based finite-element analysis of material microstructures journal, January 2001

Microstructural modeling of thermal conductivity of high burn-up mixed oxide fuel journal, January 2014

Thermal measurements and computational simulations of three-phase (CeO2–MgAl2O4–CeMgAl11O19) and four-phase (3Y-TZP–Al2O3–MgAl2O4–LaPO4) composites as surrogate inert matrix nuclear fuel journal, November 2014

MOOSE: A parallel computational framework for coupled systems of nonlinear equations journal, October 2009

Phase-field simulation of thermal conductivity in porous polycrystalline microstructures journal, August 2008

Corrigendum to “Thermophysical properties of U3Si2 to 1773 K” [J. Nucl. Mater. 464 (2015) 275–280] journal, February 2017

Effect of Fission Products and Oxygen and Carbon Impurities in (U, Pu)N on the Heat-and-Mass Transfer Coefficients and Xenon Yield journal, November 2016

Thermal conductivity of neutron irradiated Be12Ti journal, September 2003

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

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

Positions of the Oxygen Atoms in UO2.13 journal, February 1963

Magnetic properties of a mass-enhanced ferromagnet U2PtSi3 journal, February 1992

Uranium nitride-silicide advanced nuclear fuel: higher efficiency and greater safety journal, October 2018

A first-principles study on the influences of metal species Al, Zr, Mo and Tc on the mechanical properties of U 3 Si 2 journal, January 2020

Title: Fabrication and thermophysical property characterization of UN/U₃Si₂ composite fuel forms

Formation of uranium mononitride by the reaction of uranium dioxide with carbon in ammonia and a mixture of hydrogen and nitrogen— I synthesis of high purity UN
journal, December 1977

Investigation of the reaction UO2+x + PuO2 + C + N2 by thermogravimetry
journal, August 1988

Preparation of uranium nitride in the form of microspheres
journal, June 1992

The sintering of uranium mononitride
journal, October 1965

Sintering of UN as a Function of Temperature and N2 Pressure
journal, July 1971

Kinetics of the oxidation of UN and U(CO) in carbon dioxide, steam and water at elevated temperatures
journal, January 1966

Oxidation of uranium mononitride and uranium monocarbide
journal, January 1966

Hydrolysis of uranium mononitride
journal, January 1967

Oxidation of uranium mononitride
journal, September 1975

Oxidation and hydrolysis kinetic studies on UN
journal, November 1991

Dual phase MgO–ZrO2 ceramics for use in LWR inert matrix fuel
journal, June 2005

Neutronic performance of uranium nitride composite fuels in a PWR
journal, August 2014

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

Uranium silicide pellet fabrication by powder metallurgy for accident tolerant fuel evaluation and irradiation
journal, November 2015

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

Degradation of UN and UN–U ₃ Si ₂ pellets in steam environment
journal, January 2017

Development of an accident-tolerant fuel composite from uranium mononitride (UN) and uranium sesquisilicide (U3 Si2) with increased uranium loading
journal, April 2016

Fabrication and microstructural analysis of UN-U3Si2 composites for accident tolerant fuel applications
journal, August 2016

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

A new high-pressure phase of uranium nitride studied by X-ray diffraction and synchrotron radiation
journal, February 1985

Structural chemistry and magnetic behavior of binary uranium silicides
journal, April 1992

NIH Image to ImageJ: 25 years of image analysis
journal, June 2012

Improvement of the mathematical modeling of flash measurements
journal, January 2002

Flash Method of Determining Thermal Diffusivity, Heat Capacity, and Thermal Conductivity
journal, September 1961

Material property correlations for uranium mononitride
journal, May 1990

Thermophysical properties of U3Si5 to 1773 K
journal, January 2015

Material property correlations for uranium mononitride
journal, May 1990

Material property correlations for uranium mononitride
journal, May 1990

Evaluation of Rule-of-Mixtures Predictions of Thermal Expansion in Powder-Processed Ni-Al2O3 Composites
journal, October 1999

Theory of thermal expansion of composites
journal, March 1988

OOF: an image-based finite-element analysis of material microstructures
journal, January 2001

Microstructural modeling of thermal conductivity of high burn-up mixed oxide fuel
journal, January 2014

Thermal measurements and computational simulations of three-phase (CeO2–MgAl2O4–CeMgAl11O19) and four-phase (3Y-TZP–Al2O3–MgAl2O4–LaPO4) composites as surrogate inert matrix nuclear fuel
journal, November 2014

MOOSE: A parallel computational framework for coupled systems of nonlinear equations
journal, October 2009

Phase-field simulation of thermal conductivity in porous polycrystalline microstructures
journal, August 2008

Corrigendum to “Thermophysical properties of U3Si2 to 1773 K” [J. Nucl. Mater. 464 (2015) 275–280]
journal, February 2017

Effect of Fission Products and Oxygen and Carbon Impurities in (U, Pu)N on the Heat-and-Mass Transfer Coefficients and Xenon Yield
journal, November 2016

Thermal conductivity of neutron irradiated Be12Ti
journal, September 2003

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

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

Positions of the Oxygen Atoms in UO2.13
journal, February 1963

Magnetic properties of a mass-enhanced ferromagnet U2PtSi3
journal, February 1992

Uranium nitride-silicide advanced nuclear fuel: higher efficiency and greater safety
journal, October 2018

A first-principles study on the influences of metal species Al, Zr, Mo and Tc on the mechanical properties of U ₃ Si ₂
journal, January 2020