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Title: Quantification of process variables for carbothermic synthesis of UC 1-xN x fuel microspheres

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 UO 3-H 2O-C microspheres in Ar and H 2-containing gases, conversion of the resulting UO 2-C kernels to dense UO2:2UC in the same gases and vacuum, and its conversion in N 2 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 UO 2:2UC 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 N 2-H 2 mixtures to evolve HCN was shown to be quantitatively consistent with present and past experiments and the only useful application of H 2 in the entire process.
Authors:
 [1] ;  [2] ;  [2] ;  [2] ;  [2] ;  [2] ;  [2]
  1. MPI Business Solutions, Inc., Knoxville, TN (United States)
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Publication Date:
Grant/Contract Number:
AC05-00OR22725
Type:
Accepted Manuscript
Journal Name:
Journal of Nuclear Materials
Additional Journal Information:
Journal Volume: 483; Journal ID: ISSN 0022-3115
Publisher:
Elsevier
Research Org:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org:
USDOE Office of Nuclear Energy (NE)
Country of Publication:
United States
Language:
English
Subject:
11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS
OSTI Identifier:
1360046
Alternate Identifier(s):
OSTI ID: 1414021

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., Web. doi:10.1016/j.jnucmat.2016.11.006.
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. doi:10.1016/j.jnucmat.2016.11.006.
Lindemer, Terrance B., Silva, Chinthaka M., Henry, Jr, John James, McMurray, Jake W., Voit, Stewart L., Collins, Jack Lee, and Hunt, Rodney Dale. 2016. "Quantification of process variables for carbothermic synthesis of UC1-xNx fuel microspheres". United States. doi:10.1016/j.jnucmat.2016.11.006. https://www.osti.gov/servlets/purl/1360046.
@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 = {2016},
month = {11}
}