Quantification of process variables for carbothermic synthesis of UC1-xNx fuel microspheres

Lindemer, Terrance B.; Silva, Chinthaka M.; Henry, Jr, John James; McMurray, Jake W.; Voit, Stewart L.; Collins, Jack Lee; Hunt, Rodney Dale

doi:10.1016/j.jnucmat.2016.11.006

Title: Quantification of process variables for carbothermic synthesis of UC_1-xN_x fuel microspheres

Abstract

This report details the continued investigation of process variables involved in converting sol-gel-derived, urania-carbon microspheres to ~820-μm-dia. UC_1-xN_x fuel kernels in flow-through, vertical Mo and W crucibles at temperatures up to 2123 K. Experiments included calcining of air-dried UO₃-H₂O-C microspheres in Ar and H₂-containing gases, conversion of the resulting UO₂-C kernels to dense UO2:2UC in the same gases and vacuum, and its conversion in N₂ to UC_1-xN_x (x = ~0.85). The thermodynamics of the relevant reactions were applied extensively to interpret and control the process variables. Producing the precursor UO₂:2UC kernel of ~96% theoretical density was required, but its subsequent conversion to UC_1-xN_x at 2123 K was not accompanied by sintering and resulted in ~83-86% of theoretical density. Increasing the UC_1-xN_x kernel nitride component to ~0.98 in flowing N₂-H₂ mixtures to evolve HCN was shown to be quantitatively consistent with present and past experiments and the only useful application of H₂ in the entire process.

Authors:

Lindemer, Terrance B. ^[1]; Silva, Chinthaka M. ^[2]; Henry, Jr, John James ^[2]; McMurray, Jake W. ^[2]; Voit, Stewart L. ^[2]; Collins, Jack Lee ^[2]; Hunt, Rodney Dale ^[2]

MPI Business Solutions, Inc., Knoxville, TN (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

Publication Date:: Sat Nov 05 00:00:00 EDT 2016

Research Org.:: Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

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

OSTI Identifier:: 1360046

Alternate Identifier(s):: OSTI ID: 1414021

Grant/Contract Number:: AC05-00OR22725

Resource Type:: Accepted Manuscript

Journal Name:: Journal of Nuclear Materials

Additional Journal Information:: Journal Volume: 483; Journal ID: ISSN 0022-3115

Publisher:: Elsevier

Country of Publication:: United States

Language:: English

Subject:: 11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS

Citation Formats


                    Lindemer, Terrance B., Silva, Chinthaka M., Henry, Jr, John James, McMurray, Jake W., Voit, Stewart L., Collins, Jack Lee, and Hunt, Rodney Dale. Quantification of process variables for carbothermic synthesis of UC1-xNx fuel microspheres.  United States: N. p., 2016. 
Web.  doi:10.1016/j.jnucmat.2016.11.006.

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                    Lindemer, Terrance B., Silva, Chinthaka M., Henry, Jr, John James, McMurray, Jake W., Voit, Stewart L., Collins, Jack Lee, & Hunt, Rodney Dale. Quantification of process variables for carbothermic synthesis of UC1-xNx fuel microspheres.  United States.  https://doi.org/10.1016/j.jnucmat.2016.11.006

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                    Lindemer, Terrance B., Silva, Chinthaka M., Henry, Jr, John James, McMurray, Jake W., Voit, Stewart L., Collins, Jack Lee, and Hunt, Rodney Dale. Sat .  
"Quantification of process variables for carbothermic synthesis of UC1-xNx fuel microspheres".  United States.  https://doi.org/10.1016/j.jnucmat.2016.11.006.  https://www.osti.gov/servlets/purl/1360046.

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@article{osti_1360046,

  title        = {Quantification of process variables for carbothermic synthesis of UC1-xNx fuel microspheres},

  author       = {Lindemer, Terrance B. and Silva, Chinthaka M. and Henry, Jr, John James and McMurray, Jake W. and Voit, Stewart L. and Collins, Jack Lee and Hunt, Rodney Dale},

  abstractNote = {This report details the continued investigation of process variables involved in converting sol-gel-derived, urania-carbon microspheres to ~820-μm-dia. UC1-xNx fuel kernels in flow-through, vertical Mo and W crucibles at temperatures up to 2123 K. Experiments included calcining of air-dried UO3-H2O-C microspheres in Ar and H2-containing gases, conversion of the resulting UO2-C kernels to dense UO2:2UC in the same gases and vacuum, and its conversion in N2 to UC1-xNx (x = ~0.85). The thermodynamics of the relevant reactions were applied extensively to interpret and control the process variables. Producing the precursor UO2:2UC kernel of ~96% theoretical density was required, but its subsequent conversion to UC1-xNx at 2123 K was not accompanied by sintering and resulted in ~83-86% of theoretical density. Increasing the UC1-xNx kernel nitride component to ~0.98 in flowing N2-H2 mixtures to evolve HCN was shown to be quantitatively consistent with present and past experiments and the only useful application of H2 in the entire process.},

  doi          = {10.1016/j.jnucmat.2016.11.006},

  journal      = {Journal of Nuclear Materials},

  number       = ,

  volume       = 483,

  place        = {United States},

  year         = {Sat Nov 05 00:00:00 EDT 2016},

  month        = {Sat Nov 05 00:00:00 EDT 2016}

}

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Works referencing / citing this record:

Production of near‐full density uranium nitride microspheres with a hot isostatic press
journal, May 2018

McMurray, Jacob W.; Kiggans, Jim O.; Helmreich, Grant W.
Journal of the American Ceramic Society, Vol. 101, Issue 10
DOI: 10.1111/jace.15766

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Title: Quantification of process variables for carbothermic synthesis of UC1-xNx fuel microspheres

Abstract

Citation Formats

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Material property correlations for uranium mononitride journal, May 1990

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Production of Spherical UO2-UC2 for Nuclear Fuel Applications Using Thermochemical Principles journal, July 1982

Crystal habit and phase attribution of U(VI) oxides in a gelation process journal, January 1976

Reactions of uranium carbonitrides and uranium nitride with aqueous solutions of hydrochloric, sulfuric, and nitric acids journal, September 1970

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Title: Quantification of process variables for carbothermic synthesis of UC_1-xN_x fuel microspheres

Fabrication and characterization of fully ceramic microencapsulated fuels
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journal, August 2012

Process Variables in the Preparation of UN Microspheres
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Preparation of uranium nitride in the form of microspheres
journal, June 1992

Kinetics of the carbothermic synthesis of uranium mononitride microspheres
journal, November 1991

Kinetics and mechanism of UO2 + C reaction for preparation
journal, June 1994

Carbothermic synthesis of 820μm uranium nitride kernels: Literature review, thermodynamics, analysis, and related experiments
journal, May 2014

Preparation of spherical, dense uranium fuel kernels with carbon
journal, January 2007

Preparation of UC0.07−0.10N0.90−0.93 spheres for TRISO coated fuel particles
journal, May 2014

Characteristics of uranium carbonitride microparticles synthesized using different reaction conditions
journal, November 2014

Material property correlations for uranium mononitride
journal, May 1990

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

Fabrication of (U, Pu)N fuel pellets
journal, December 1989

Production of Spherical UO2-UC2 for Nuclear Fuel Applications Using Thermochemical Principles
journal, July 1982

Crystal habit and phase attribution of U(VI) oxides in a gelation process
journal, January 1976

Reactions of uranium carbonitrides and uranium nitride with aqueous solutions of hydrochloric, sulfuric, and nitric acids
journal, September 1970

Investigations on uranium carbonitrides (I)
journal, June 1975

Kinetics of the UO ₂ -C-N ₂ Reaction at 1700°C
journal, December 1972

Uranium nitride as LWR TRISO fuel: Thermodynamic modeling of U–C–N
journal, August 2012

Phase Relations in the System Uranium-Carbon-Oxygen
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The compound energy formalism
journal, May 2001

Thermodynamic modelling of advanced oxide and carbide nuclear fuels: Description of the U–Pu–O–C systems
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