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Title: Gas Phase Chemical Evolution of Uranium, Aluminum, and Iron Oxides

We use a recently developed plasma-flow reactor to experimentally investigate the formation of oxide nanoparticles from gas phase metal atoms during oxidation, homogeneous nucleation, condensation, and agglomeration processes. Gas phase uranium, aluminum, and iron atoms were cooled from 5000 K to 1000 K over short-time scales (Δt < 30 ms) at atmospheric pressures in the presence of excess oxygen. In-situ emission spectroscopy is used to measure the variation in monoxide/atomic emission intensity ratios as a function of temperature and oxygen fugacity. Condensed oxide nanoparticles are collected inside the reactor for ex-situ analyses using scanning and transmission electron microscopy (SEM, TEM) to determine their structural compositions and sizes. A chemical kinetics model is also developed to describe the gas phase reactions of iron and aluminum metals. The resulting sizes and forms of the crystalline nanoparticles (FeO-wustite, eta-Al 2O 3, UO 2, and alpha-UO 3) depend on the thermodynamic properties, kinetically-limited gas phase chemical reactions, and local redox conditions. This work shows the nucleation and growth of metal oxide particles in rapidly-cooling gas is closely coupled to the kinetically-controlled chemical pathways for vapor-phase oxide formation.
Authors:
 [1] ; ORCiD logo [1] ;  [1] ;  [1] ;  [1] ;  [1] ;  [2] ;  [1] ;  [1] ;  [1]
  1. Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
  2. Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States); Politecnico di Milano (Italy)
Publication Date:
Report Number(s):
LLNL-JRNL-741152
Journal ID: ISSN 2045-2322; 895505
Grant/Contract Number:
AC52-07NA27344
Type:
Published Article
Journal Name:
Scientific Reports
Additional Journal Information:
Journal Volume: 8; Journal Issue: 1; Journal ID: ISSN 2045-2322
Publisher:
Nature Publishing Group
Research Org:
Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
Sponsoring Org:
USDOE National Nuclear Security Administration (NNSA)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
OSTI Identifier:
1459036
Alternate Identifier(s):
OSTI ID: 1463831

Koroglu, Batikan, Wagnon, Scott, Dai, Zurong, Crowhurst, Jonathan C., Armstrong, Michael R., Weisz, David, Mehl, Marco, Zaug, Joseph M., Radousky, Harry B., and Rose, Timothy P.. Gas Phase Chemical Evolution of Uranium, Aluminum, and Iron Oxides. United States: N. p., Web. doi:10.1038/s41598-018-28674-6.
Koroglu, Batikan, Wagnon, Scott, Dai, Zurong, Crowhurst, Jonathan C., Armstrong, Michael R., Weisz, David, Mehl, Marco, Zaug, Joseph M., Radousky, Harry B., & Rose, Timothy P.. Gas Phase Chemical Evolution of Uranium, Aluminum, and Iron Oxides. United States. doi:10.1038/s41598-018-28674-6.
Koroglu, Batikan, Wagnon, Scott, Dai, Zurong, Crowhurst, Jonathan C., Armstrong, Michael R., Weisz, David, Mehl, Marco, Zaug, Joseph M., Radousky, Harry B., and Rose, Timothy P.. 2018. "Gas Phase Chemical Evolution of Uranium, Aluminum, and Iron Oxides". United States. doi:10.1038/s41598-018-28674-6.
@article{osti_1459036,
title = {Gas Phase Chemical Evolution of Uranium, Aluminum, and Iron Oxides},
author = {Koroglu, Batikan and Wagnon, Scott and Dai, Zurong and Crowhurst, Jonathan C. and Armstrong, Michael R. and Weisz, David and Mehl, Marco and Zaug, Joseph M. and Radousky, Harry B. and Rose, Timothy P.},
abstractNote = {We use a recently developed plasma-flow reactor to experimentally investigate the formation of oxide nanoparticles from gas phase metal atoms during oxidation, homogeneous nucleation, condensation, and agglomeration processes. Gas phase uranium, aluminum, and iron atoms were cooled from 5000 K to 1000 K over short-time scales (Δt < 30 ms) at atmospheric pressures in the presence of excess oxygen. In-situ emission spectroscopy is used to measure the variation in monoxide/atomic emission intensity ratios as a function of temperature and oxygen fugacity. Condensed oxide nanoparticles are collected inside the reactor for ex-situ analyses using scanning and transmission electron microscopy (SEM, TEM) to determine their structural compositions and sizes. A chemical kinetics model is also developed to describe the gas phase reactions of iron and aluminum metals. The resulting sizes and forms of the crystalline nanoparticles (FeO-wustite, eta-Al2O3, UO2, and alpha-UO3) depend on the thermodynamic properties, kinetically-limited gas phase chemical reactions, and local redox conditions. This work shows the nucleation and growth of metal oxide particles in rapidly-cooling gas is closely coupled to the kinetically-controlled chemical pathways for vapor-phase oxide formation.},
doi = {10.1038/s41598-018-28674-6},
journal = {Scientific Reports},
number = 1,
volume = 8,
place = {United States},
year = {2018},
month = {7}
}