The effect of oxygen concentration on the speciation of laser ablated uranium
Abstract
In order to model the fate and transport of particles following a nuclear explosion, there must first be an understanding of individual physical and chemical processes that affect particle formation. One interaction pertinent to fireball chemistry and resultant debris formation is that between uranium and oxygen. In this study, we use laser ablation of uranium metal in different concentrations of oxygen gas, either 16O2 or 18O2, to determine the influence of oxygen on rapidly cooling uranium. Analysis of recovered particulates using infrared absorption and Raman spectroscopies indicate that the micrometer-sized particulates are predominantly amorphous UOx (am-UOx, where 3 ≤ x ≤ 4) and UO2 after ablation in 1 atm of pure O2 and a 1% O2/Ar mixture, respectively. Energy dispersive X-ray spectroscopy (EDS) of particulates formed in pure O2 suggest an O/U ratio of ~ 3.7, consistent with the vibrational spectroscopy analysis. Both am-UOx and UO2 particulates convert to α-U3O8 when heated. Lastly, experiments performed in 18O2 environments show the formation of 18O-substituted uranium oxides; vibrational frequencies for am-U18Ox are reported for the first time. When compared to literature, this work shows that cooling timescales can affect the structural composition of uranium oxides (i.e., crystalline vs. amorphous). This indicator canmore »
- Authors:
- Publication Date:
- Research Org.:
- Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States); Univ. of Michigan, Ann Arbor, MI (United States)
- Sponsoring Org.:
- USDOE National Nuclear Security Administration (NNSA)
- OSTI Identifier:
- 1847967
- Alternate Identifier(s):
- OSTI ID: 1860897; OSTI ID: 1864567
- Report Number(s):
- LLNL-JRNL-826652
Journal ID: ISSN 2045-2322; 4030; PII: 7834
- Grant/Contract Number:
- 20-SI-006; HDTRA1-20-2-0001; NE000863; DGE 1256260; AC52-07NA27344; NA0003920
- Resource Type:
- Published Article
- Journal Name:
- Scientific Reports
- Additional Journal Information:
- Journal Name: Scientific Reports Journal Volume: 12 Journal Issue: 1; Journal ID: ISSN 2045-2322
- Publisher:
- Nature Publishing Group
- Country of Publication:
- United Kingdom
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEAR CHEMISTRY; Analytical chemistry; Physical chemistry
Citation Formats
Burton, Mark A., Auner, Alex W., Crowhurst, Jonathan C., Boone, Peter S., Finney, Lauren A., Weisz, David G., Koroglu, Batikan, Jovanovic, Igor, Radousky, Harry B., and Knight, Kim B. The effect of oxygen concentration on the speciation of laser ablated uranium. United Kingdom: N. p., 2022.
Web. doi:10.1038/s41598-022-07834-9.
Burton, Mark A., Auner, Alex W., Crowhurst, Jonathan C., Boone, Peter S., Finney, Lauren A., Weisz, David G., Koroglu, Batikan, Jovanovic, Igor, Radousky, Harry B., & Knight, Kim B. The effect of oxygen concentration on the speciation of laser ablated uranium. United Kingdom. https://doi.org/10.1038/s41598-022-07834-9
Burton, Mark A., Auner, Alex W., Crowhurst, Jonathan C., Boone, Peter S., Finney, Lauren A., Weisz, David G., Koroglu, Batikan, Jovanovic, Igor, Radousky, Harry B., and Knight, Kim B. Mon .
"The effect of oxygen concentration on the speciation of laser ablated uranium". United Kingdom. https://doi.org/10.1038/s41598-022-07834-9.
@article{osti_1847967,
title = {The effect of oxygen concentration on the speciation of laser ablated uranium},
author = {Burton, Mark A. and Auner, Alex W. and Crowhurst, Jonathan C. and Boone, Peter S. and Finney, Lauren A. and Weisz, David G. and Koroglu, Batikan and Jovanovic, Igor and Radousky, Harry B. and Knight, Kim B.},
abstractNote = {In order to model the fate and transport of particles following a nuclear explosion, there must first be an understanding of individual physical and chemical processes that affect particle formation. One interaction pertinent to fireball chemistry and resultant debris formation is that between uranium and oxygen. In this study, we use laser ablation of uranium metal in different concentrations of oxygen gas, either 16O2 or 18O2, to determine the influence of oxygen on rapidly cooling uranium. Analysis of recovered particulates using infrared absorption and Raman spectroscopies indicate that the micrometer-sized particulates are predominantly amorphous UOx (am-UOx, where 3 ≤ x ≤ 4) and UO2 after ablation in 1 atm of pure O2 and a 1% O2/Ar mixture, respectively. Energy dispersive X-ray spectroscopy (EDS) of particulates formed in pure O2 suggest an O/U ratio of ~ 3.7, consistent with the vibrational spectroscopy analysis. Both am-UOx and UO2 particulates convert to α-U3O8 when heated. Lastly, experiments performed in 18O2 environments show the formation of 18O-substituted uranium oxides; vibrational frequencies for am-U18Ox are reported for the first time. When compared to literature, this work shows that cooling timescales can affect the structural composition of uranium oxides (i.e., crystalline vs. amorphous). This indicator can be used in current models of nuclear explosions to improve our predicative capabilities of chemical speciation.},
doi = {10.1038/s41598-022-07834-9},
journal = {Scientific Reports},
number = 1,
volume = 12,
place = {United Kingdom},
year = {Mon Mar 07 00:00:00 EST 2022},
month = {Mon Mar 07 00:00:00 EST 2022}
}
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