Use of boiled hexamethylenetetramine and urea to increase the porosity of cerium dioxide microspheres formed in the internal gelation process
Abstract
Cerium dioxide (CeO2) is a commonly used simulant for plutonium dioxide and for plutonium (Pu) in a mixed uranium (U) and Pu oxide [(U, Pu)O2] in nuclear fuel development. This effort developed CeO2 microspheres with different porosities and diameters for use in a crush-strength study. The internal gelation technique has produced CeO2 microspheres with limited initial porosity. When an equal molar solution of urea and hexamethylenetetramine (HMTA) is gently boiling for 1 hr and used in the gelation process, the crystallite size and porosity of mixed U and thorium oxide microspheres and the (U, Pu)O2 microspheres increased significantly. In this study with cerium, the combination of ammonium cerium nitrate and 1-h boiled HMTA-urea failed to produce a stable feed broth. However, when the 1-h heated HMTA-urea was combined with unheated HMTA-urea in 1 to 3 volume ratio or the boiling time of the HMTA-urea was reduced to 15-20 min, a stable solution of HMTA, urea, and Ce was formed at 273 K. This new Ce solution produced CeO2 microspheres with much higher initial porosities. Intermediate porosities were possible when the heated HMTA/urea was aged prior to use.
- Authors:
-
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- Publication Date:
- Research Org.:
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- Sponsoring Org.:
- USDOE
- OSTI Identifier:
- 1408648
- Alternate Identifier(s):
- OSTI ID: 1396929
- Grant/Contract Number:
- AC05-00OR22725
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Nuclear Materials
- Additional Journal Information:
- Journal Volume: 492; 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; Cerium oxide spheres; Internal gelation
Citation Formats
Hunt, R. D., Collins, J. L., and Cowell, B. S. Use of boiled hexamethylenetetramine and urea to increase the porosity of cerium dioxide microspheres formed in the internal gelation process. United States: N. p., 2017.
Web. doi:10.1016/j.jnucmat.2017.04.061.
Hunt, R. D., Collins, J. L., & Cowell, B. S. Use of boiled hexamethylenetetramine and urea to increase the porosity of cerium dioxide microspheres formed in the internal gelation process. United States. https://doi.org/10.1016/j.jnucmat.2017.04.061
Hunt, R. D., Collins, J. L., and Cowell, B. S. Sat .
"Use of boiled hexamethylenetetramine and urea to increase the porosity of cerium dioxide microspheres formed in the internal gelation process". United States. https://doi.org/10.1016/j.jnucmat.2017.04.061. https://www.osti.gov/servlets/purl/1408648.
@article{osti_1408648,
title = {Use of boiled hexamethylenetetramine and urea to increase the porosity of cerium dioxide microspheres formed in the internal gelation process},
author = {Hunt, R. D. and Collins, J. L. and Cowell, B. S.},
abstractNote = {Cerium dioxide (CeO2) is a commonly used simulant for plutonium dioxide and for plutonium (Pu) in a mixed uranium (U) and Pu oxide [(U, Pu)O2] in nuclear fuel development. This effort developed CeO2 microspheres with different porosities and diameters for use in a crush-strength study. The internal gelation technique has produced CeO2 microspheres with limited initial porosity. When an equal molar solution of urea and hexamethylenetetramine (HMTA) is gently boiling for 1 hr and used in the gelation process, the crystallite size and porosity of mixed U and thorium oxide microspheres and the (U, Pu)O2 microspheres increased significantly. In this study with cerium, the combination of ammonium cerium nitrate and 1-h boiled HMTA-urea failed to produce a stable feed broth. However, when the 1-h heated HMTA-urea was combined with unheated HMTA-urea in 1 to 3 volume ratio or the boiling time of the HMTA-urea was reduced to 15-20 min, a stable solution of HMTA, urea, and Ce was formed at 273 K. This new Ce solution produced CeO2 microspheres with much higher initial porosities. Intermediate porosities were possible when the heated HMTA/urea was aged prior to use.},
doi = {10.1016/j.jnucmat.2017.04.061},
journal = {Journal of Nuclear Materials},
number = C,
volume = 492,
place = {United States},
year = {Sat May 13 00:00:00 EDT 2017},
month = {Sat May 13 00:00:00 EDT 2017}
}
Web of Science
Works referenced in this record:
Fabrication of size-controlled CeO 2 microparticles by a microfluidic sol–gel process as an analog preparation of ceramic nuclear fuel particles
journal, August 2013
- Ye, Bin; Miao, Ji-Lang; Li, Jiao-Long
- Journal of Nuclear Science and Technology, Vol. 50, Issue 8
Fabrication of dense (Th,U)O2 pellets through microspheres impregnation technique
journal, November 2008
- Pai, Rajesh V.; Dehadraya, J. V.; Bhattacharya, Shovit
- Journal of Nuclear Materials, Vol. 381, Issue 3
Studies on preparation of (U0.47,Pu0.53)O2 microspheres by internal gelation process
journal, March 2013
- Kumar, Ashok; Radhakrishna, J.; Kumar, N.
- Journal of Nuclear Materials, Vol. 434, Issue 1-3
The Basic Chemistry Involved in the Internal-Gelation Method of Precipitating Uranium as Determined by pH Measurements
journal, January 1987
- Collins, J. L.; Lloyd, M. H.; Fellows, R. L.
- Radiochimica Acta, Vol. 42, Issue 3
Uranium kernel formation via internal gelation
journal, January 2004
- Hunt, Rodney D.; Collins, Jack L.
- Radiochimica Acta, Vol. 92, Issue 12
Treatment techniques to prevent cracking of amorphous microspheres made by the internal gelation process
journal, October 2010
- Hunt, R. D.; Montgomery, F. C.; Collins, J. L.
- Journal of Nuclear Materials, Vol. 405, Issue 2
Works referencing / citing this record:
Preparation of cerium dioxide microspheres by internal gelation with cerium citrate as precursor
journal, March 2019
- Ding, Xueqiang; Ma, Jingtao; Zhou, Xiangwen
- Journal of Sol-Gel Science and Technology, Vol. 90, Issue 2
Fabrication of CeO2–Nd2O3 microspheres by internal gelation process using M(OH)m and [MCit∙xH2O] (M=Ce3+, Ce4+, and Nd3+) as precursors
journal, July 2019
- Ding, Xueqiang; Ma, Jingtao; Zhou, Xiangwen
- Journal of Sol-Gel Science and Technology, Vol. 92, Issue 1