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

Abstract

Abstract 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 (∆t < 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 2 O 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:
; ORCiD logo; ; ; ; ; ; ; ;
Publication Date:
Research Org.:
Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)
Sponsoring Org.:
USDOE National Nuclear Security Administration (NNSA)
OSTI Identifier:
1459036
Alternate Identifier(s):
OSTI ID: 1463831
Report Number(s):
LLNL-JRNL-741152
Journal ID: ISSN 2045-2322; 10451; PII: 28674
Grant/Contract Number:  
AC52-07NA27344
Resource Type:
Published Article
Journal Name:
Scientific Reports
Additional Journal Information:
Journal Name: Scientific Reports Journal Volume: 8 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

Citation Formats

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 Kingdom: N. p., 2018. Web. doi:10.1038/s41598-018-28674-6.
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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 Kingdom. https://doi.org/10.1038/s41598-018-28674-6
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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. Wed . "Gas Phase Chemical Evolution of Uranium, Aluminum, and Iron Oxides". United Kingdom. https://doi.org/10.1038/s41598-018-28674-6.
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@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 = {Abstract 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 (∆t < 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 2 O 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.},
doi = {10.1038/s41598-018-28674-6},
journal = {Scientific Reports},
number = 1,
volume = 8,
place = {United Kingdom},
year = {Wed Jul 11 00:00:00 EDT 2018},
month = {Wed Jul 11 00:00:00 EDT 2018}
}
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https://doi.org/10.1038/s41598-018-28674-6
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margin-top: 0.5em; padding-left: 0; line-height:1.8em;"> <li> <span style="color:#5C7B2D;"> Opila, Elizabeth J.; Myers, Dwight L.</span> </li> <li> Journal of the American Ceramic Society, Vol. 87, Issue 9</li> <li> <span class="text-muted related-url">DOI: <a href="https://doi.org/10.1111/j.1551-2916.2004.01701.x" class="text-muted" target="_blank" rel="noopener noreferrer">10.1111/j.1551-2916.2004.01701.x<span class="fa fa-external-link" aria-hidden="true"></span></a></span> </li> </ul> <hr/> </div> <div> <h2 class="title" style="margin-bottom:0;" data-apporder=""> <a href="https://doi.org/10.1103/PhysRevB.71.184106" target="_blank" rel="noopener noreferrer" class="name">Vibrational spectroscopy of <math display="inline"> <mrow> <mi>Fe</mi> <mrow> <msub> <mrow> <mo>(</mo> <mi>OH</mi> <mo>)</mo> </mrow> <mn>2</mn> </msub> </mrow> </mrow> </math> at high pressure: Behavior of the O-H bond<span class="fa fa-external-link" aria-hidden="true"></span></a> <small class="text-muted" style="text-transform:uppercase; font-size:0.75rem;"><br/> <span class="type">journal</span>, <span class="date" data-date="2005-05-01">May 2005</span></small> </h2> <ul class="small references-list" style="list-style-type:none; margin-top: 0.5em; padding-left: 0; line-height:1.8em;"> <li> <span style="color:#5C7B2D;"> Speziale, Sergio; Jeanloz, Raymond; Milner, Alla</span> </li> <li> Physical Review B, Vol. 71, Issue 18</li> <li> <span class="text-muted related-url">DOI: <a href="https://doi.org/10.1103/PhysRevB.71.184106" class="text-muted" target="_blank" rel="noopener noreferrer">10.1103/PhysRevB.71.184106<span class="fa fa-external-link" aria-hidden="true"></span></a></span> </li> </ul> <hr/> </div> <div> <h2 class="title" style="margin-bottom:0;" data-apporder=""> <a href="https://doi.org/10.1080/02786829708965459" target="_blank" rel="noopener noreferrer" class="name">Simultaneous Particle and Molecule Modeling (SPAMM): An Approach for Combining Sectional Aerosol Equations and Elementary Gas-Phase Reactions<span class="fa fa-external-link" aria-hidden="true"></span></a> <small class="text-muted" style="text-transform:uppercase; font-size:0.75rem;"><br/> <span class="type">journal</span>, <span class="date" data-date="1997-01-01">January 1997</span></small> </h2> <ul class="small references-list" style="list-style-type:none; margin-top: 0.5em; padding-left: 0; line-height:1.8em;"> <li> <span style="color:#5C7B2D;"> Pope, Christopher J.; Howard, Jack B.</span> </li> <li> Aerosol Science and Technology, Vol. 27, Issue 1</li> <li> <span class="text-muted related-url">DOI: <a href="https://doi.org/10.1080/02786829708965459" class="text-muted" target="_blank" rel="noopener noreferrer">10.1080/02786829708965459<span class="fa fa-external-link" aria-hidden="true"></span></a></span> </li> </ul> <hr/> </div> <div> <h2 class="title" style="margin-bottom:0;" data-apporder=""> <a href="https://doi.org/10.1038/srep43852" target="_blank" rel="noopener noreferrer" class="name">Standoff Detection of Uranium and its Isotopes by Femtosecond Filament Laser Ablation Molecular Isotopic Spectrometry<span class="fa fa-external-link" aria-hidden="true"></span></a> <small class="text-muted" style="text-transform:uppercase; font-size:0.75rem;"><br/> <span class="type">journal</span>, <span class="date" data-date="2017-03-08">March 2017</span></small> </h2> <ul class="small references-list" style="list-style-type:none; margin-top: 0.5em; padding-left: 0; line-height:1.8em;"> <li> <span style="color:#5C7B2D;"> Hartig, Kyle C.; Ghebregziabher, Isaac; Jovanovic, Igor</span> </li> <li> Scientific Reports, Vol. 7, Issue 1</li> <li> <span class="text-muted related-url">DOI: <a href="https://doi.org/10.1038/srep43852" class="text-muted" target="_blank" rel="noopener noreferrer">10.1038/srep43852<span class="fa fa-external-link" aria-hidden="true"></span></a></span> </li> </ul> <hr/> </div> <div> <h2 class="title" style="margin-bottom:0;" data-apporder=""> <a href="https://doi.org/10.1366/13-07066" target="_blank" rel="noopener noreferrer" class="name">Line Selection and Parameter Optimization for Trace Analysis of Uranium in Glass Matrices by Laser-Induced Breakdown Spectroscopy (LIBS)<span class="fa fa-external-link" aria-hidden="true"></span></a> <small class="text-muted" style="text-transform:uppercase; font-size:0.75rem;"><br/> <span class="type">journal</span>, <span class="date" data-date="2013-11-01">November 2013</span></small> </h2> <ul class="small references-list" style="list-style-type:none; margin-top: 0.5em; padding-left: 0; line-height:1.8em;"> <li> <span style="color:#5C7B2D;"> Choi, Inhee; Chan, George C. -Y.; Mao, Xianglei</span> </li> <li> Applied Spectroscopy, Vol. 67, Issue 11</li> <li> <span class="text-muted related-url">DOI: <a href="https://doi.org/10.1366/13-07066" class="text-muted" target="_blank" rel="noopener noreferrer">10.1366/13-07066<span class="fa fa-external-link" aria-hidden="true"></span></a></span> </li> </ul> <hr/> </div> <div> <h2 class="title" style="margin-bottom:0;" data-apporder=""> <a href="https://doi.org/10.1021/jp066579q" target="_blank" rel="noopener noreferrer" class="name">Detailed Kinetic Modeling of Iron Nanoparticle Synthesis from the Decomposition of Fe(CO) <sub>5</sub><span class="fa fa-external-link" aria-hidden="true"></span></a> <small class="text-muted" style="text-transform:uppercase; font-size:0.75rem;"><br/> <span class="type">journal</span>, <span class="date" data-date="2007-04-01">April 2007</span></small> </h2> <ul class="small references-list" style="list-style-type:none; margin-top: 0.5em; padding-left: 0; line-height:1.8em;"> <li> <span style="color:#5C7B2D;"> Wen, John Z.; Goldsmith, C. Franklin; Ashcraft, Robert W.</span> </li> <li> The Journal of Physical Chemistry C, Vol. 111, Issue 15</li> <li> <span class="text-muted related-url">DOI: <a href="https://doi.org/10.1021/jp066579q" class="text-muted" target="_blank" rel="noopener noreferrer">10.1021/jp066579q<span class="fa fa-external-link" aria-hidden="true"></span></a></span> </li> </ul> <hr/> </div> <div> <h2 class="title" style="margin-bottom:0;" data-apporder=""> <a href="https://doi.org/10.1016/0584-8547(92)80072-O" target="_blank" rel="noopener noreferrer" class="name">Isocontour maps of electron temperature, electron number density and gas kinetic temperature in the Ar inductively coupled plasma obtained by laser-light Thomson and Rayleigh scattering<span class="fa fa-external-link" aria-hidden="true"></span></a> <small class="text-muted" style="text-transform:uppercase; font-size:0.75rem;"><br/> <span class="type">journal</span>, <span class="date" data-date="1992-06-01">June 1992</span></small> </h2> <ul class="small references-list" style="list-style-type:none; margin-top: 0.5em; padding-left: 0; line-height:1.8em;"> <li> <span style="color:#5C7B2D;"> Huang, Mao; Hanselman, D. S.; Yang, Pengyuan</span> </li> <li> Spectrochimica Acta Part B: Atomic Spectroscopy, Vol. 47, Issue 6</li> <li> <span class="text-muted related-url">DOI: <a href="https://doi.org/10.1016/0584-8547(92)80072-O" class="text-muted" target="_blank" rel="noopener noreferrer">10.1016/0584-8547(92)80072-O<span class="fa fa-external-link" aria-hidden="true"></span></a></span> </li> </ul> <hr/> </div> <div> <h2 class="title" style="margin-bottom:0;" data-apporder=""> <a href="https://doi.org/10.1007/s11090-004-8837-2" target="_blank" rel="noopener noreferrer" class="name">Kinetic Modeling of the Decomposition of Carbon Tetrachloride in Thermal Plasma<span class="fa fa-external-link" aria-hidden="true"></span></a> <small class="text-muted" style="text-transform:uppercase; font-size:0.75rem;"><br/> <span class="type">journal</span>, <span class="date" data-date="2005-04-01">April 2005</span></small> </h2> <ul class="small references-list" style="list-style-type:none; margin-top: 0.5em; padding-left: 0; line-height:1.8em;"> <li> <span style="color:#5C7B2D;"> Kov�cs, Tam�s; Tur�nyi, Tam�s; F�glein, Katalin</span> </li> <li> Plasma Chemistry and Plasma Processing, Vol. 25, Issue 2</li> <li> <span class="text-muted related-url">DOI: <a href="https://doi.org/10.1007/s11090-004-8837-2" class="text-muted" target="_blank" rel="noopener noreferrer">10.1007/s11090-004-8837-2<span class="fa fa-external-link" aria-hidden="true"></span></a></span> </li> </ul> <hr/> </div> <div> <h2 class="title" style="margin-bottom:0;" data-apporder=""> <a href="https://doi.org/10.1016/j.sab.2015.12.006" target="_blank" rel="noopener noreferrer" class="name">Hybrid interferometric/dispersive atomic spectroscopy of laser-induced uranium plasma<span class="fa fa-external-link" aria-hidden="true"></span></a> <small class="text-muted" style="text-transform:uppercase; font-size:0.75rem;"><br/> <span class="type">journal</span>, <span class="date" data-date="2016-02-01">February 2016</span></small> </h2> <ul class="small references-list" style="list-style-type:none; margin-top: 0.5em; padding-left: 0; line-height:1.8em;"> <li> <span style="color:#5C7B2D;"> Morgan, Phyllis K.; Scott, Jill R.; Jovanovic, Igor</span> </li> <li> Spectrochimica Acta Part B: Atomic Spectroscopy, Vol. 116</li> <li> <span class="text-muted related-url">DOI: <a href="https://doi.org/10.1016/j.sab.2015.12.006" class="text-muted" target="_blank" rel="noopener noreferrer">10.1016/j.sab.2015.12.006<span class="fa fa-external-link" aria-hidden="true"></span></a></span> </li> </ul> <hr/> </div> <div> <h2 class="title" style="margin-bottom:0;" data-apporder=""> <a href="https://doi.org/10.1016/0009-2614(73)87070-8" target="_blank" rel="noopener noreferrer" class="name">The infrared spectrum of matrix-isolated uranium oxide vapor species<span class="fa fa-external-link" aria-hidden="true"></span></a> <small class="text-muted" style="text-transform:uppercase; font-size:0.75rem;"><br/> <span class="type">journal</span>, <span class="date" data-date="1973-01-01">January 1973</span></small> </h2> <ul class="small references-list" style="list-style-type:none; margin-top: 0.5em; padding-left: 0; line-height:1.8em;"> <li> <span style="color:#5C7B2D;"> Gabelnick, S. D.; Reedy, G. T.; Chasanov, M. G.</span> </li> <li> Chemical Physics Letters, Vol. 19, Issue 1</li> <li> <span class="text-muted related-url">DOI: <a href="https://doi.org/10.1016/0009-2614(73)87070-8" class="text-muted" target="_blank" rel="noopener noreferrer">10.1016/0009-2614(73)87070-8<span class="fa fa-external-link" aria-hidden="true"></span></a></span> </li> </ul> <hr/> </div> <div> <h2 class="title" style="margin-bottom:0;" data-apporder=""> <a href="https://doi.org/10.1366/000370294775268893" target="_blank" rel="noopener noreferrer" class="name">Characterization of Binary Uranium Oxides by Infrared Spectroscopy<span class="fa fa-external-link" aria-hidden="true"></span></a> <small class="text-muted" style="text-transform:uppercase; font-size:0.75rem;"><br/> <span class="type">journal</span>, <span class="date" data-date="1994-04-01">April 1994</span></small> </h2> <ul class="small references-list" style="list-style-type:none; margin-top: 0.5em; padding-left: 0; line-height:1.8em;"> <li> <span style="color:#5C7B2D;"> Allen, Geoffrey C.; Holmes, Nigel R.</span> </li> <li> Applied Spectroscopy, Vol. 48, Issue 4</li> <li> <span class="text-muted related-url">DOI: <a href="https://doi.org/10.1366/000370294775268893" class="text-muted" target="_blank" rel="noopener noreferrer">10.1366/000370294775268893<span class="fa fa-external-link" aria-hidden="true"></span></a></span> </li> </ul> <hr/> </div> <div> <h2 class="title" style="margin-bottom:0;" data-apporder=""> <a href="https://doi.org/10.1016/j.sab.2015.05.011" target="_blank" rel="noopener noreferrer" class="name">Boron- and iron-bearing molecules in laser-induced plasma<span class="fa fa-external-link" aria-hidden="true"></span></a> <small class="text-muted" style="text-transform:uppercase; font-size:0.75rem;"><br/> <span class="type">journal</span>, <span class="date" data-date="2015-08-01">August 2015</span></small> </h2> <ul class="small references-list" style="list-style-type:none; margin-top: 0.5em; padding-left: 0; line-height:1.8em;"> <li> <span style="color:#5C7B2D;"> Gaft, M.; Nagli, L.; Eliezer, N.</span> </li> <li> Spectrochimica Acta Part B: Atomic Spectroscopy, Vol. 110</li> <li> <span class="text-muted related-url">DOI: <a href="https://doi.org/10.1016/j.sab.2015.05.011" class="text-muted" target="_blank" rel="noopener noreferrer">10.1016/j.sab.2015.05.011<span class="fa fa-external-link" aria-hidden="true"></span></a></span> </li> </ul> <hr/> </div> <div> <h2 class="title" style="margin-bottom:0;" data-apporder=""> <a href="https://doi.org/10.1063/1.1762015" target="_blank" rel="noopener noreferrer" class="name">Condensation and Electrical Conduction in Metallic Vapors<span class="fa fa-external-link" aria-hidden="true"></span></a> <small class="text-muted" style="text-transform:uppercase; font-size:0.75rem;"><br/> <span class="type">journal</span>, <span class="date" data-date="1967-01-01">January 1967</span></small> </h2> <ul class="small references-list" style="list-style-type:none; margin-top: 0.5em; padding-left: 0; line-height:1.8em;"> <li> <span style="color:#5C7B2D;"> Solbes, Albert</span> </li> <li> Physics of Fluids, Vol. 10, Issue 10</li> <li> <span class="text-muted related-url">DOI: <a href="https://doi.org/10.1063/1.1762015" class="text-muted" target="_blank" rel="noopener noreferrer">10.1063/1.1762015<span class="fa fa-external-link" aria-hidden="true"></span></a></span> </li> </ul> <hr/> </div> </div> <div class="pagination-container small"> <a class="pure-button prev page" href="#" rel="prev"><span class="sr-only">Previous Page</span><span class="fa fa-angle-left"></span></a> <ul class="pagination d-inline-block" style="padding-left:.2em;"></ul> <a class="pure-button next page" href="#" rel="next"><span class="sr-only">Next Page</span><span class="fa fa-angle-right"></span></a> </div> </div> </div> <div class="col-sm-3 order-sm-3"> <ul class="nav nav-stacked"> <li class="active"><a href="" class="reference-type-filter tab-nav" data-tab="biblio-references" data-filter="type" data-pattern="*"><span class="fa fa-angle-right"></span> All References</a></li> <li class="small" style="margin-left:.75em; 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list-style-type: none;"> <li> <div class="article item document" itemprop="itemListElement" itemscope itemtype="http://schema.org/WebPage"><meta itemprop="position" content="1" /><div class="item-info"> <h2 class="title" itemprop="name headline"><a href="/pages/biblio/1656961-experimental-investigation-uranium-volatility-during-vapor-condensation" itemprop="url">Experimental Investigation of Uranium Volatility during Vapor Condensation</a></h2> <div class="metadata"> <small class="text-muted" style="text-transform:uppercase;display:block;line-height:2.5em;">Journal Article</small><span class="authors"> <span class="author">Koroglu, Batikan</span> ; <span class="author">Dai, Zurong</span> ; <span class="author">Finko, Mikhail</span> ; <span class="author">...</span> <span class="text-muted pubdata"> - Analytical Chemistry</span> </span> </div> <div class="abstract">The predictive models that describe the fate and transport of radioactive materials in the atmosphere following a nuclear incident (explosion or reactor accident) assume that uranium-bearing particulates would attain chemical equilibrium during vapor condensation. Here, we show that kinetically driven processes in a system of rapidly decreasing temperature can result in substantial deviations from chemical equilibrium. This can cause uranium to condense out in oxidation states (e.g., UO<sub>3</sub> vs UO<sub>2</sub>) that have different vapor pressures, significantly affecting uranium transport. To demonstrate this, we synthesized uranium oxide nanoparticles using a flow reactor under controlled conditions of temperature, pressure, and oxygen concentration.<a href='#' onclick='$(this).hide().next().show().next().show();return false;' style='margin-left:10px;'>more »</a><span style='display:none;'> The atomized chemical reactants passing through an inductively coupled plasma cool from ~5000 to 1000 K within milliseconds and form nanoparticles inside a flow reactor. The ex situ analysis of particulates by transmission electron microscopy revealed 2–10 nm crystallites of fcc-UO<sub>2</sub> or α-UO<sub>3</sub> depending on the amount of oxygen in the system. α-UO<sub>3</sub> is the least thermodynamically preferred polymorph of UO<sub>3</sub>. The absence of stable uranium oxides with intermediate stoichiometries (e.g., U<sub>3</sub>O<sub>8</sub>) and sensitivity of the uranium oxidation states to local redox conditions highlight the importance of in situ measurements at high temperatures. Therefore, we developed a laser-based diagnostic to detect uranium oxide particles as they are formed inside the flow reactor. Our in situ measurements allowed us to quantify the changes in the number densities of the uranium oxide nanoparticles (e.g., UO<sub>3</sub>) as a function of oxygen gas concentration. Our results indicate that uranium can prefer to be in metastable crystal forms (i.e., α-UO<sub>3</sub>) that have higher vapor pressures than the refractory form (i.e., UO<sub>2</sub>) depending on the oxygen abundance in the surrounding environment. This demonstrates that the equilibrium processes may not dominate during rapid condensation processes, and thus kinetic models are required to fully describe uranium transport subsequent to nuclear incidents.</span><a href='#' onclick='$(this).hide().prev().hide().prev().show();return false;' style='margin-left:10px;display:none;'>« less</a></div><div class="metadata-links small clearfix text-muted" style="margin-top:15px;"> <span class="fa fa-book text-muted" aria-hidden="true"></span> Cited by 11<div class="pure-menu pure-menu-horizontal pull-right" style="width:unset;"> <ul class="pure-menu-list"> <li class="pure-menu-item"><span class="item-info-ftlink"><a class="misc doi-link " href="https://doi.org/10.1021/acs.analchem.9b05562" target="_blank" rel="noopener" title="Link to document DOI" data-ostiid="1656961" data-product-type="Journal Article" data-product-subtype="AM" >https://doi.org/10.1021/acs.analchem.9b05562</a></span></li> <li class="pure-menu-item"><span class="item-info-ftlink"><a class="misc fulltext-link " href="/pages/servlets/purl/1656961" title="Link to document media" target="_blank" rel="noopener" data-ostiid="1656961" data-product-type="Journal Article" data-product-subtype="AM" >Full Text Available</a></span></li> </ul> </div> </div> </div> <div class="clearfix"></div> </div> </li> <li> <div class="article item document" itemprop="itemListElement" itemscope itemtype="http://schema.org/WebPage"><meta itemprop="position" content="2" /><div class="item-info"> <h2 class="title" itemprop="name headline"><a href="/pages/biblio/1897689-vapor-phase-aggregation-cerium-oxide-nanoparticles-rapidly-cooling-plasma" itemprop="url">Vapor-Phase Aggregation of Cerium Oxide Nanoparticles in a Rapidly Cooling Plasma</a></h2> <div class="metadata"> <small class="text-muted" style="text-transform:uppercase;display:block;line-height:2.5em;">Journal Article</small><span class="authors"> <span class="author">Rodriguez, Kate</span> ; <span class="author">Koroglu, Batikan</span> ; <span class="author">Hammons, Joshua</span> ; <span class="author">...</span> <span class="text-muted pubdata"> - ACS Earth and Space Chemistry</span> </span> </div> <div class="abstract">Local conditions, such as temperature and oxygen availability, have a pronounced effect on the formation and evolution of fallout following a nuclear explosion. While the behavior of nuclear-relevant materials such as uranium has begun to be explored under a wider range of environments, little is known about the behavior of plutonium. Here, using cerium as a surrogate, we track the vapor-phase aggregation of cerium oxide nanoparticles created in a plasma flow reactor under conditions of controlled temperature at two different oxygen fugacities. In situ optical emission spectroscopy is used to measure the variations in the spectral intensity of atomic and<a href='#' onclick='$(this).hide().next().show().next().show();return false;' style='margin-left:10px;'>more »</a><span style='display:none;'> molecular species with temperature and oxygen content. We find that the relative rate of gas-phase oxidation of cerium is highly dependent on both temperature and local redox conditions within the flow reactor, to the extent that doubling the oxygen availability effectively doubles the amount of vapor-phase cerium monoxide at high temperatures (>2000 K). Condensed cerium oxide nanoparticles are also collected and analyzed ex situ via transmission electron microscopy and grazing-incidence small-angle X-ray scattering to determine their elemental composition, crystal structure, and size distribution. The size and morphology of the condensed nanoparticles are independent of local redox conditions, forming the same crystal type with the same size distribution regardless of oxygen availability. Postcondensation particle evolution, however, is found to be predominantly driven by temperature, with the average particle size increasing as particles cool and subsequently aggregate. These results expand our understanding of the chemical and physical behavior of refractory oxides that form during the early stages of fallout formation.</span><a href='#' onclick='$(this).hide().prev().hide().prev().show();return false;' style='margin-left:10px;display:none;'>« less</a></div><div class="metadata-links small clearfix text-muted" style="margin-top:15px;"> <div class="pure-menu pure-menu-horizontal pull-right" style="width:unset;"> <ul class="pure-menu-list"> <li class="pure-menu-item"><span class="item-info-ftlink"><a class="misc doi-link " href="https://doi.org/10.1021/acsearthspacechem.2c00073" target="_blank" rel="noopener" title="Link to document DOI" data-ostiid="1897689" data-product-type="Journal Article" data-product-subtype="AM" >https://doi.org/10.1021/acsearthspacechem.2c00073</a></span></li> <li class="pure-menu-item"><span class="item-info-ftlink"><a class="misc fulltext-link " href="/pages/servlets/purl/1897689" title="Link to document media" target="_blank" rel="noopener" data-ostiid="1897689" data-product-type="Journal Article" data-product-subtype="AM" >Full Text Available</a></span></li> </ul> </div> </div> </div> <div class="clearfix"></div> </div> </li> <li> <div class="article item document" itemprop="itemListElement" itemscope itemtype="http://schema.org/WebPage"><meta itemprop="position" content="3" /><div class="item-info"> <h2 class="title" itemprop="name headline"><a href="/pages/biblio/2005042-influence-cooling-rate-condensation-iron-aluminum-uranium-oxide-nanoparticles" itemprop="url">The influence of cooling rate on condensation of iron, aluminum, and uranium oxide nanoparticles</a></h2> <div class="metadata"> <small class="text-muted" style="text-transform:uppercase;display:block;line-height:2.5em;">Journal Article</small><span class="authors"> <span class="author">Koroglu, Batikan</span> ; <span class="author">Finko, Mikhail</span> ; <span class="author">Saggese, Chiara</span> ; <span class="author">...</span> <span class="text-muted pubdata"> - Journal of Aerosol Science</span> </span> </div> <div class="abstract">Fundamental observations of particle size distributions are needed to develop models that predict the fate and transport of radioactive materials in the atmosphere following a nuclear incident. The extent of material transport is influenced by the time scales of particle formation processes (e.g., condensation, coagulation). In this study, we investigated the influence of cooling time scales on size distributions of uranium, aluminum, and iron oxide particles that are synthesized separately under identical run conditions inside the controlled environment of an argon plasma flow reactor. Two distinct temperature distributions are imposed along the flow reactor by varying the argon flow rate<a href='#' onclick='$(this).hide().next().show().next().show();return false;' style='margin-left:10px;'>more »</a><span style='display:none;'> downstream of the plasma torch. The vaporized reactants of uranium, aluminum, and iron are cooled from about 5000K to 1000K before they are collected on silicon wafers for ex situ scanning electron microscope analysis. The microscope images show that the sizes of the largest aluminum and iron oxide particles heavily depend on the cooling time scales, whereas significant size variation with cooling rate is not observed for uranium oxide particles. In addition, the size distribution of aluminum oxide particles exhibits the broadest range among all three metal oxides studied. We performed simulations of particle size distributions using a kinetic model that couples gas phase oxidation chemistry with particle formation processes, including nucleation, condensation, and coagulation. The model results demonstrate the strong sensitivity of particle size distribution to different cooling histories (i.e., temperature vs residence time) along the flow reactor. In conclusion, the kinetic model also helps identify directions for future research to improve the predictions.</span><a href='#' onclick='$(this).hide().prev().hide().prev().show();return false;' style='margin-left:10px;display:none;'>« less</a></div><div class="metadata-links small clearfix text-muted" style="margin-top:15px;"> <div class="pure-menu pure-menu-horizontal pull-right" style="width:unset;"> <ul class="pure-menu-list"> <li class="pure-menu-item"><span class="item-info-ftlink"><a class="misc doi-link " href="https://doi.org/10.1016/j.jaerosci.2022.105959" target="_blank" rel="noopener" title="Link to document DOI" data-ostiid="2005042" data-product-type="Journal Article" data-product-subtype="AM" >https://doi.org/10.1016/j.jaerosci.2022.105959</a></span></li> <li class="pure-menu-item"><span class="item-info-ftlink"><a class="misc fulltext-link " href="/pages/servlets/purl/2005042" title="Link to document media" target="_blank" rel="noopener" data-ostiid="2005042" data-product-type="Journal Article" data-product-subtype="AM" >Full Text Available</a></span></li> </ul> </div> </div> </div> <div class="clearfix"></div> </div> </li> <li> <div class="article item document" itemprop="itemListElement" itemscope itemtype="http://schema.org/WebPage"><meta itemprop="position" content="5" /><div class="item-info"> <h2 class="title" itemprop="name headline"><a href="/pages/biblio/1882239-synthesis-stability-eightcoordinated-fe-highpressure-phase-implications-mantle-structure-superearths" itemprop="url">Synthesis and Stability of an Eight‐Coordinated Fe <sub>3</sub> O <sub>4</sub> High‐Pressure Phase: Implications for the Mantle Structure of Super‐Earths</a></h2> <div class="metadata"> <small class="text-muted" style="text-transform:uppercase;display:block;line-height:2.5em;">Journal Article</small><span class="authors"> <span class="author">Zurkowski, C. C.</span> ; <span class="author">Yang, J.</span> ; <span class="author">Chariton, S.</span> ; <span class="author">...</span> <span class="text-muted pubdata"> - Journal of Geophysical Research. Planets</span> </span> </div> <div class="abstract">Abstract Super‐Earths ranging up to 10 Earth masses (M <sub>E</sub> ) with Earth‐like density are common among the observed exoplanets thus far, but their measured masses and radii do not uniquely elucidate their internal structure. Exploring the phase transitions in the Mg‐silicates that define the mantle‐structure of super‐Earths is critical to characterizing their interiors, yet the relevant terapascal conditions are experimentally challenging for direct structural analysis. Here we investigated the crystal chemistry of Fe <sub>3</sub> O <sub>4</sub> as a low‐pressure analog to Mg <sub>2</sub> SiO <sub>4</sub> between 45–115 GPa and up to 3000 K using powder and single crystal X‐ray diffraction in<a href='#' onclick='$(this).hide().next().show().next().show();return false;' style='margin-left:10px;'>more »</a><span style='display:none;'> the laser‐heated diamond anvil cell. Between 60–115 GPa and above 2000 K, Fe <sub>3</sub> O <sub>4</sub> adopts an 8‐fold coordinated Th <sub>3</sub> P <sub>4</sub> ‐type structure ( I ‐43d, Z  = 4) with disordered Fe <sup>2+</sup> and Fe <sup>3+</sup> into one metal site. This Fe‐oxide phase is isostructural with that predicted for Mg <sub>2</sub> SiO <sub>4</sub> above 500 GPa in super‐Earth mantles and suggests that Mg <sub>2</sub> SiO <sub>4</sub> can incorporate both ferric and ferrous iron at these conditions. The pressure‐volume behavior observed in this 8‐fold coordinated Fe <sub>3</sub> O <sub>4</sub> indicates a maximum 4% density increase across the 6‐ to 8‐fold coordination transition in the analog Mg‐silicate. Reassessment of the FeO—Fe <sub>3</sub> O <sub>4</sub> fugacity buffer considering the Fe <sub>3</sub> O <sub>4</sub> phase relationships identified in this study reveals that increasing pressure and temperature to 120 GPa and 3000 K in Earth and planetary mantles drives iron toward oxidation.</span><a href='#' onclick='$(this).hide().prev().hide().prev().show();return false;' style='margin-left:10px;display:none;'>« less</a></div><div class="metadata-links small clearfix text-muted" style="margin-top:15px;"> <div class="pure-menu pure-menu-horizontal pull-right" style="width:unset;"> <ul class="pure-menu-list"> <li class="pure-menu-item"><span class="item-info-ftlink"><a class="misc doi-link " href="https://doi.org/10.1029/2022JE007344" target="_blank" rel="noopener" title="Link to document DOI" data-ostiid="1882239" data-product-type="Journal Article" data-product-subtype="PA" >https://doi.org/10.1029/2022JE007344</a></span></li> </ul> </div> </div> </div> <div class="clearfix"></div> </div> </li> <li> <div class="article item document" itemprop="itemListElement" itemscope itemtype="http://schema.org/WebPage"><meta itemprop="position" content="6" /><div class="item-info"> <h2 class="title" itemprop="name headline"><a href="/pages/biblio/1894772-hyperstoichiometric-uranium-dioxides-rapid-synthesis-irradiation-induced-structural-changes" itemprop="url">Hyperstoichiometric Uranium Dioxides: Rapid Synthesis and Irradiation-Induced Structural Changes</a></h2> <div class="metadata"> <small class="text-muted" style="text-transform:uppercase;display:block;line-height:2.5em;">Journal Article</small><span class="authors"> <span class="author">Roach, Jordan M.</span> ; <span class="author">Manukyan, Khachatur V.</span> ; <span class="author">Majumdar, Ashabari</span> ; <span class="author">...</span> <span class="text-muted pubdata"> - Inorganic Chemistry</span> </span> </div> <div class="abstract">Uranium dioxide (UO<sub>2</sub>), the primary fuel for commercial nuclear reactors, incorporates excess oxygen forming a series of hyperstoichiometric oxides. Thin layers of these oxides, such as UO<sub>2.12</sub>, form readily on the fuel surface and influence its properties, performance, and potentially geologic disposal. This work reports a rapid and straightforward combustion process in uranyl nitrate–glycine–water solutions to prepare UO<sub>2.12</sub> nanomaterials and thin films. We also report on the investigation of the structural changes induced in the material by irradiation. Despite the simple processing aspects, the combustion synthesis of UO<sub>2.12</sub> has a sophisticated chemical mechanism involving several exothermic steps. Raman spectroscopy and<a href='#' onclick='$(this).hide().next().show().next().show();return false;' style='margin-left:10px;'>more »</a><span style='display:none;'> single-crystal X-ray diffraction (XRD) measurements reveal the formation of a complex compound containing the uranyl moiety, glycine, H<sub>2</sub>O, and NO<sub>3</sub><sup>–</sup> groups in reactive solutions and dried combustion precursors. Combustion diagnostic methods, gas-phase mass spectroscopy, differential scanning calorimetry (DSC), and extracted activation energies from DSC measurements show that the rate-limiting step of the process is the reaction of ammonia with nitrogen oxides formed from the decomposition of glycine and uranyl nitrate, respectively. However, the exothermic decomposition of the complex compound determines the maximum temperature of the process. In situ transmission electron microscopy (TEM) imaging and electron diffraction measurements show that the decomposition of the complex compound directly produces UO<sub>2</sub>. The incorporation of oxygen at the cooling stage of the combustion process is responsible for the formation of UO<sub>2.12</sub>. Spin coating of the solutions and brief annealing at 670 K allow the deposition of uniform films of UO<sub>2.12</sub> with thicknesses up to 300 nm on an aluminum substrate. Irradiation of films with Ar<sup>2+</sup> ions (1.7 MeV energy, a fluence of up to 1 × 10<sup>17</sup> ions/cm<sup>2</sup>) shows unusual defect-simulated grain growth and enhanced chemical mixing of UO<sub>2.12</sub> with the substrate due to the high uranium ion diffusion in films. As a result, the method described in this work allows the preparation of actinide oxide targets for fundamental nuclear science research and studies associated with stockpile stewardship.</span><a href='#' onclick='$(this).hide().prev().hide().prev().show();return false;' style='margin-left:10px;display:none;'>« less</a></div><div class="metadata-links small clearfix text-muted" style="margin-top:15px;"> <div class="pure-menu pure-menu-horizontal pull-right" style="width:unset;"> <ul class="pure-menu-list"> <li class="pure-menu-item"><span class="item-info-ftlink"><a class="misc doi-link " href="https://doi.org/10.1021/acs.inorgchem.1c02736" target="_blank" rel="noopener" title="Link to document DOI" data-ostiid="1894772" data-product-type="Journal Article" data-product-subtype="AM" >https://doi.org/10.1021/acs.inorgchem.1c02736</a></span></li> <li class="pure-menu-item"><span class="item-info-ftlink"><a class="misc fulltext-link " href="/pages/servlets/purl/1894772" title="Link to document media" target="_blank" rel="noopener" data-ostiid="1894772" data-product-type="Journal Article" data-product-subtype="AM" >Full Text Available</a></span></li> </ul> </div> </div> </div> <div class="clearfix"></div> </div> </li> </ul> </aside> </div> </section> </div> <div class="col-sm-3 order-sm-3"> <ul class="nav nav-stacked"> <li class="active"><a class="tab-nav disabled" data-tab="related" style="color: #636c72 !important; 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