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Title: Pyrolytic Carbon Coating Effects on Oxide and Carbide Kernels Intended for Nuclear Fuel Applications

Abstract

The coating of nuclear fuel kernels with pyrolytic carbon (PyC) is a well-understood practice dating back over half a century. In spite of decades of studies related to these coatings, no study has yet investigated the effect of the PyC deposition coating process on the kernels themselves. In this study, the composition and crystallographic phase of kernel materials were observed to change after exposure to the thermal and chemical environment of PyC coating process. Specifically, the coating process increased the fraction of high carbon content phase within carbide microsphere kernels, with W 2C containing microspheres driven towards WC, and UC containing microspheres driven towards UC 2. Oxide microspheres consisted of a mixture of two crystalline phases. The monoclinic phase within yttria-stabilized zirconia microspheres was eliminated by the coating process resulting in a purely tetragonal phase. Hafnium oxide microspheres were more stable showing no detectable change in composition or crystal structure after coating.

Authors:
ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1];  [1];  [1];  [1]; ORCiD logo [1]; ORCiD logo [1];  [1];  [1];  [1]; ORCiD logo [1]
  1. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Publication Date:
Research Org.:
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Sponsoring Org.:
USDOE Laboratory Directed Research and Development (LDRD) Program
OSTI Identifier:
1544671
Report Number(s):
LA-UR-18-20776
Journal ID: ISSN 0029-5450
Grant/Contract Number:  
89233218CNA000001
Resource Type:
Accepted Manuscript
Journal Name:
Nuclear Technology
Additional Journal Information:
Journal Name: Nuclear Technology; Journal ID: ISSN 0029-5450
Publisher:
Taylor & Francis - formerly American Nuclear Society (ANS)
Country of Publication:
United States
Language:
English
Subject:
11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Pyrolytic carbon; nuclear fuel; chemical vapor deposition

Citation Formats

Beaux, Miles Frank II, Vodnik, Douglas R., Peterson, Reuben James, Bennett, Bryan L., Hubbard, Kevin Mark, Patterson, Brian M., Goettee, Jeffrey D., Jurney, James D., King, Graham M., Smith, Alice Iulia, Tegtmeier, Eric Lee, Luther, Erik Paul, Dasari, Venkateswara Rao, Devlin, David James, and Usov, Igor Olegovich. Pyrolytic Carbon Coating Effects on Oxide and Carbide Kernels Intended for Nuclear Fuel Applications. United States: N. p., 2019. Web. doi:10.1080/00295450.2019.1618683.
Beaux, Miles Frank II, Vodnik, Douglas R., Peterson, Reuben James, Bennett, Bryan L., Hubbard, Kevin Mark, Patterson, Brian M., Goettee, Jeffrey D., Jurney, James D., King, Graham M., Smith, Alice Iulia, Tegtmeier, Eric Lee, Luther, Erik Paul, Dasari, Venkateswara Rao, Devlin, David James, & Usov, Igor Olegovich. Pyrolytic Carbon Coating Effects on Oxide and Carbide Kernels Intended for Nuclear Fuel Applications. United States. doi:10.1080/00295450.2019.1618683.
Beaux, Miles Frank II, Vodnik, Douglas R., Peterson, Reuben James, Bennett, Bryan L., Hubbard, Kevin Mark, Patterson, Brian M., Goettee, Jeffrey D., Jurney, James D., King, Graham M., Smith, Alice Iulia, Tegtmeier, Eric Lee, Luther, Erik Paul, Dasari, Venkateswara Rao, Devlin, David James, and Usov, Igor Olegovich. Fri . "Pyrolytic Carbon Coating Effects on Oxide and Carbide Kernels Intended for Nuclear Fuel Applications". United States. doi:10.1080/00295450.2019.1618683.
@article{osti_1544671,
title = {Pyrolytic Carbon Coating Effects on Oxide and Carbide Kernels Intended for Nuclear Fuel Applications},
author = {Beaux, Miles Frank II and Vodnik, Douglas R. and Peterson, Reuben James and Bennett, Bryan L. and Hubbard, Kevin Mark and Patterson, Brian M. and Goettee, Jeffrey D. and Jurney, James D. and King, Graham M. and Smith, Alice Iulia and Tegtmeier, Eric Lee and Luther, Erik Paul and Dasari, Venkateswara Rao and Devlin, David James and Usov, Igor Olegovich},
abstractNote = {The coating of nuclear fuel kernels with pyrolytic carbon (PyC) is a well-understood practice dating back over half a century. In spite of decades of studies related to these coatings, no study has yet investigated the effect of the PyC deposition coating process on the kernels themselves. In this study, the composition and crystallographic phase of kernel materials were observed to change after exposure to the thermal and chemical environment of PyC coating process. Specifically, the coating process increased the fraction of high carbon content phase within carbide microsphere kernels, with W2C containing microspheres driven towards WC, and UC containing microspheres driven towards UC2. Oxide microspheres consisted of a mixture of two crystalline phases. The monoclinic phase within yttria-stabilized zirconia microspheres was eliminated by the coating process resulting in a purely tetragonal phase. Hafnium oxide microspheres were more stable showing no detectable change in composition or crystal structure after coating.},
doi = {10.1080/00295450.2019.1618683},
journal = {Nuclear Technology},
number = ,
volume = ,
place = {United States},
year = {2019},
month = {6}
}

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Works referenced in this record:

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    Works referencing / citing this record:

    The influence of deposition temperature on the microstructure of isotropic pyrocarbon obtained by hot-wall chemical vapor deposition
    journal, January 2011


    The structure of pyrolytic carbon deposited in a fluidized bed
    journal, July 1965


    Variation in the crystallinity of carbons deposited in fluidized beds
    journal, October 1965


    Deformation and fracture of pyrolytic carbons deposited in a fluidized bed
    journal, February 1966


    Structure and properties of pyrolytic carbons prepared in a fluidized bed between 1900° and 2400°C
    journal, July 1966


    Pyrolytic-carbon coatings deposited from methane fluid beds
    journal, December 1967


    Comments on a unifying coating parameter
    journal, February 1967


    Pyrolytic carbons deposited in fluidized beds at 1200 to 1400°c from various hydrocarbons
    journal, October 1968


    Basal planes annealing behaviour of pyrolytic carbons prepared in a fluidized bed
    journal, October 1973


    Ceramic coated particle nuclear fuels
    journal, January 1964


    Thermodynamic properties of uranium carbides
    journal, February 1967


    Über die bildung des U2C3
    journal, October 1968


    Studies on the U-C constitutional diagram between UC and UC2
    journal, August 1969


    Structure and mechanical properties of isotropic pyrolytic carbons deposited below 1600 °C
    journal, January 1971


    Thermally induced structural modifications in pyrolytic carbons and their relationship with the deposition temperature
    journal, October 1974


    Quantitative aspects of the fluidized bed deposition of pyrocarbon
    journal, April 1977


    Some theoretical aspects of pyrocarbon formation in the gas phase during hydrocarbon pyrolysis
    journal, January 1977


    Fluidized bed chemical vapor deposition of pyrolytic carbon – II. Effect of deposition conditions on anisotropy
    journal, January 2009


    Fluidized bed chemical vapor deposition of pyrolytic carbon – I. Effect of deposition conditions on microstructure
    journal, February 2009


    Structure and mechanical properties of pyrolytic carbon produced by fluidized bed chemical vapor deposition
    journal, November 2008


    Fabrication and characterization of driver-fuel particles, designed-to-fail fuel particles, and fuel compacts for the US AGR-3/4 irradiation test
    journal, May 2014


    Chemical vapor deposition of Mo tubes for fuel cladding applications
    journal, March 2018


    Rate analysis of chemical vapor deposition by use of the thin tubular reactor
    journal, March 2006


    Modeling of Chemical Vapor Deposition of Pyrolytic Carbon in a Gas-Spouted Bed Reactor
    journal, December 2011

    • Mollick, Palash Kumar; Sathiyamoorthy, Dakshinamoorthy; Rao, Pandugula Thirmaleshwar
    • Industrial & Engineering Chemistry Research, Vol. 50, Issue 23
    • DOI: 10.1021/ie2009636

    Dissociation Pressure of Uranium Dicarbide
    journal, March 1962

    • Leitnaker, James M.; Witteman, Willard G.
    • The Journal of Chemical Physics, Vol. 36, Issue 6
    • DOI: 10.1063/1.1732762

    Formation of U 2 C 3 from UC 2 by Heating under Stress
    journal, July 1973

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    • Journal of Nuclear Science and Technology, Vol. 10, Issue 7
    • DOI: 10.1080/18811248.1973.9733044

    Diffusionless Phase Transformations in Zirconia and Hafnia
    journal, September 1963