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Title: Facile incorporation of technetium into magnetite, magnesioferrite, and hematite by formation of ferrous nitrate in situ: precursors to iron oxide nuclear waste forms

Abstract

The fission product,99Tc, presents significant challenges to the long-term disposal of nuclear waste due to its long half-life, high fission yield, and to the environmental mobility of pertechnetate (TcO4–), the stable Tc species in aerobic environments. Here, the migration of 99Tc from disposal sites can potentially be prevented by incorporating it into durable waste forms based on environmentally stable minerals.

Authors:
ORCiD logo [1]; ORCiD logo [2]
+ Show Author Affiliations
  1. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  2. Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Environmental Management (EM)
OSTI Identifier:
1550810
Alternate Identifier(s):
OSTI ID: 1460584
Grant/Contract Number:  
AC02-05CH11231; AC02-76SF00515; AC05-76RL01830
Resource Type:
Accepted Manuscript
Journal Name:
Dalton Transactions
Additional Journal Information:
Journal Volume: 47; Journal Issue: 30; Journal ID: ISSN 1477-9226
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE WASTES FROM NUCLEAR FACILITIES

Citation Formats

Lukens, Wayne W., and Saslow, Sarah A. Facile incorporation of technetium into magnetite, magnesioferrite, and hematite by formation of ferrous nitrate in situ: precursors to iron oxide nuclear waste forms. United States: N. p., 2018. Web. doi:10.1039/c8dt01356j.
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Lukens, Wayne W., & Saslow, Sarah A. Facile incorporation of technetium into magnetite, magnesioferrite, and hematite by formation of ferrous nitrate in situ: precursors to iron oxide nuclear waste forms. United States. doi:https://doi.org/10.1039/c8dt01356j
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Lukens, Wayne W., and Saslow, Sarah A. Tue . "Facile incorporation of technetium into magnetite, magnesioferrite, and hematite by formation of ferrous nitrate in situ: precursors to iron oxide nuclear waste forms". United States. doi:https://doi.org/10.1039/c8dt01356j. https://www.osti.gov/servlets/purl/1550810.
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@article{osti_1550810,
title = {Facile incorporation of technetium into magnetite, magnesioferrite, and hematite by formation of ferrous nitrate in situ: precursors to iron oxide nuclear waste forms},
author = {Lukens, Wayne W. and Saslow, Sarah A.},
abstractNote = {The fission product,99Tc, presents significant challenges to the long-term disposal of nuclear waste due to its long half-life, high fission yield, and to the environmental mobility of pertechnetate (TcO4–), the stable Tc species in aerobic environments. Here, the migration of 99Tc from disposal sites can potentially be prevented by incorporating it into durable waste forms based on environmentally stable minerals.},
doi = {10.1039/c8dt01356j},
journal = {Dalton Transactions},
number = 30,
volume = 47,
place = {United States},
year = {2018},
month = {7}
}
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DOI:  https://doi.org/10.1039/c8dt01356j
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float:none;">[ × clear filter / sort ]</a> </div> </form> </div> </div> </div> </section> <section id="biblio-related" class="tab-content tab-content-sec " data-tab="biblio"> <div class="row"> <div class="col-sm-9 order-sm-9"> <section id="biblio-similar" class="tab-content tab-content-sec active" data-tab="related"> <div class="padding"> <p class="lead text-muted" style="font-size: 18px; margin-top:0px;">Similar Records in DOE PAGES and OSTI.GOV collections:</p> <aside> <ul class="item-list" itemscope itemtype="http://schema.org/ItemList" style="padding-left:0; list-style-type: none;"> <li> <div class="article item document" itemprop="itemListElement" itemscope itemtype="http://schema.org/WebPage"><meta itemprop="position" content="0" /><div class="item-info"> <h2 class="title" itemprop="name headline"><a href="/biblio/1485476-facile-incorporation-technetium-magnetite-magnesioferrite-hematite-formation-ferrous-nitrate-situ-precursors-iron-oxide-nuclear-waste-forms" itemprop="url">Facile incorporation of technetium into magnetite, magnesioferrite, and hematite by formation of ferrous nitrate <em>in situ</em> : precursors to iron oxide nuclear waste forms</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">Lukens, Wayne W.</span> ; <span class="author">Saslow, Sarah A.</span> <span class="text-muted pubdata"> - Dalton Transactions</span> </span> </div> <div class="abstract">Technetium (<sup>99</sup>Tc) is a problematic fission product for the long-term disposal of nuclear waste due to its long half-life, high fission yield, and to the environmental mobility of pertechnetate, the stable Tc species in aerobic environments. One approach to preventing <sup>99</sup>Tc contamination is using durable waste forms based on environmentally stable natural analogs such as hematite (-Fe<sub>2</sub>O<sub>3</sub>) or magnesioferrite (MgFe<sub>2</sub>O<sub>4</sub>). The incorporation of Tc into hematite, magnesioferrite, and magnetite (Fe<sub>3</sub>O<sub>4</sub>) by means of simple, aqueous chemistry is presented starting from TcO<sub>4</sub><sup>-</sup> in 5 M nitric acid. A combination of X-ray diffraction and X-ray absorption fine structure spectroscopy reveals that Tc(IV)<a href='#' onclick='$(this).hide().next().show().next().show();return false;' style='margin-left:10px;'>more »</a><span style='display:none;'> replaces Fe(III) within the iron oxide structures. Following incorporation, Tc doped samples were suspended in deionized water under aerobic conditions, and the release rate of Tc under these conditions was determined. The results of this work show that Tc leaches more quickly from Fe<sub>3</sub>O<sub>4</sub> than from -Fe<sub>2</sub>O<sub>3</sub> or MgFe<sub>2</sub>O<sub>4</sub>.</span><a href='#' onclick='$(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">DOI: <a class="misc doi-link " href="https://doi.org/10.1039/C8DT01356J" target="_blank" rel="noopener" title="Link to document DOI" data-ostiid="1485476" data-product-type="Journal Article" data-product-subtype="AC" >https://doi.org/10.1039/C8DT01356J</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/1482510-incorporation-technetium-spinel-ferrites" itemprop="url">Incorporation of Technetium into Spinel Ferrites</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">Lukens, Wayne W.</span> ; <span class="author">Magnani, Nicola</span> ; <span class="author">Tyliszczak, Tolek</span> ; <span class="author">...</span> <span class="text-muted pubdata"> - Environmental Science and Technology</span> </span> </div> <div class="abstract">Technetium (<sup>99</sup>Tc) is a problematic fission product for the long-term disposal of nuclear waste due to its long half-life, high fission yield, and to the environmental mobility of pertechnetate, the stable species in aerobic environments. One approach to preventing <sup>99</sup>Tc contamination is using sufficiently durable waste forms. We report the incorporation of technetium into a family of synthetic spinel ferrites that have environmentally durable natural analogs. A combination of X-ray diffraction, X-ray absorption fine structure spectroscopy, and chemical analysis reveals that Tc(IV) replaces Fe(III) in octahedral sites and illustrates how the resulting charge mismatch is balanced. When a large excess<a href='#' onclick='$(this).hide().next().show().next().show();return false;' style='margin-left:10px;'>more »</a><span style='display:none;'> of divalent metal ions is present, the charge is predominantly balanced by substitution of Fe(III) by M(II). When a large excess of divalent metal ions is absent, the charge is largely balanced by creation of vacancies among the Fe(III) sites (maghemitization). In most samples, Tc is present in Tc-rich regions rather than being homogeneously distributed.</span><a href='#' onclick='$(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 20<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">DOI: <a class="misc doi-link " href="https://doi.org/10.1021/acs.est.6b04209" target="_blank" rel="noopener" title="Link to document DOI" data-ostiid="1482510" data-product-type="Journal Article" data-product-subtype="AM" >https://doi.org/10.1021/acs.est.6b04209</a></span></li> <li class="pure-menu-item"><span class="item-info-ftlink"><a class="misc fulltext-link " href="/pages/servlets/purl/1482510" title="Link to document media" target="_blank" rel="noopener" data-ostiid="1482510" 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/1482527-aqueous-synthesis-technetium-doped-titanium-dioxide-direct-oxidation-titanium-powder-precursor-ceramic-nuclear-waste-forms" itemprop="url">Aqueous Synthesis of Technetium-Doped Titanium Dioxide by Direct Oxidation of Titanium Powder, a Precursor for Ceramic Nuclear Waste Forms</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">Lukens, Wayne W.</span> ; <span class="author">Saslow, Sarah A.</span> <span class="text-muted pubdata"> - Chemistry of Materials</span> </span> </div> <div class="abstract">Technetium-99 (Tc) is a problematic fission product that complicates the long-term disposal of nuclear waste due to its long half-life, high fission yield, and the environmental mobility of pertechnetate, its stable form in aerobic environments. One approach to preventing Tc contamination is through incorporation into durable waste forms based on weathering-resistant minerals such as rutile (titanium dioxide). Here, the incorporation of technetium into titanium dioxide by means of simple, aqueous chemistry - direct oxidation of titanium powder in the presence of ammonium fluoride - is achieved. X-ray absorption fine structure spectroscopy and diffuse reflectance spectroscopy indicate that Tc(IV) replaces Ti(IV)<a href='#' onclick='$(this).hide().next().show().next().show();return false;' style='margin-left:10px;'>more »</a><span style='display:none;'> within the structure. Rather than being incorporated as isolated Tc(IV) ions, Tc is present as pairs of edge-sharing Tc(IV) octahedra similar to molecular Tc(IV) complexes such as [(H<sub>2</sub>EDTA)TcIV](μ-O)<sub>2</sub>. Technetium-doped TiO<sub>2</sub> was suspended in deionized water under aerobic conditions, and the Tc leached under these conditions was followed for 8 months. The normalized release rate of Tc (LR<sub>Tc</sub>) from the TiO<sub>2</sub> particles is low (3 × 10<sup>-6</sup>g m<sup>-2</sup>d<sup>-1</sup>), which illustrates the potential utility of TiO<sub>2</sub> as waste form. However, the small size of the as-prepared TiO<sub>2</sub> nanoparticles results in an estimated retention of Tc of 10<sup>4</sup> years, which is only a fraction of the half-life of Tc (2.1 × 10<sup>5</sup> years).</span><a href='#' onclick='$(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 5<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">DOI: <a class="misc doi-link " href="https://doi.org/10.1021/acs.chemmater.7b03567" target="_blank" rel="noopener" title="Link to document DOI" data-ostiid="1482527" data-product-type="Journal Article" data-product-subtype="AM" >https://doi.org/10.1021/acs.chemmater.7b03567</a></span></li> <li class="pure-menu-item"><span class="item-info-ftlink"><a class="misc fulltext-link " href="/pages/servlets/purl/1482527" title="Link to document media" target="_blank" rel="noopener" data-ostiid="1482527" 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="4" /><div class="item-info"> <h2 class="title" itemprop="name headline"><a href="/biblio/1422329-aqueous-synthesis-technetium-doped-titanium-dioxide-direct-oxidation-titanium-powder-precursor-ceramic-nuclear-waste-forms" itemprop="url">Aqueous Synthesis of Technetium-Doped Titanium Dioxide by Direct Oxidation of Titanium Powder, a Precursor for Ceramic Nuclear Waste Forms</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">Lukens, Wayne W.</span> ; <span class="author">Saslow, Sarah A.</span> <span class="text-muted pubdata"> - Chemistry of Materials</span> </span> </div> <div class="abstract">Technetium-99 (Tc) is a problematic fission product that complicates the long-term disposal of nuclear waste due to its long half-life, high fission yield, and the environmental mobility of pertechnetate, its stable form in aerobic environments. One approach to preventing Tc contamination is through incorporation into durable waste forms based on weathering-resistant minerals such as rutile (titanium dioxide). Here, the incorporation of technetium into titanium dioxide by means of simple, aqueous chemistry is presented. X-ray absorption fine structure spectroscopy and diffuse reflectance spectroscopy indicate that Tc(IV) replaces Ti(IV) within the structure. Rather than being incorporated as isolated Tc(IV) ions, Tc is<a href='#' onclick='$(this).hide().next().show().next().show();return false;' style='margin-left:10px;'>more »</a><span style='display:none;'> present as pairs of edge-sharing Tc(IV) octahedra similar to molecular Tc(IV) complexes such as [(H2EDTA)TcIV](u-O)2. Technetium-doped TiO2 was suspended in deionized water under aerobic conditions, and the Tc leached under these conditions was followed for 8 months. The normalized release rate of Tc (LRTc) from the TiO2 particles is low (3×10-6 g m-2 d-1), which illustrates the potential utility of TiO2 as waste form. However, the small size of the as-prepared TiO2 nanoparticles results in estimated retention of Tc for 104 years, which is only a fraction of the half-life of Tc (2×10-5 years).</span><a href='#' onclick='$(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">DOI: <a class="misc doi-link " href="https://doi.org/10.1021/acs.chemmater.7b03567" target="_blank" rel="noopener" title="Link to document DOI" data-ostiid="1422329" data-product-type="Journal Article" data-product-subtype="AC" >https://doi.org/10.1021/acs.chemmater.7b03567</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="/biblio/22822640-technetium-incorporation-glass-hanford-tank-waste-treatment-immobilization-plant" itemprop="url">Technetium incorporation in glass for the Hanford Tank Waste treatment and immobilization plant - 15066</a></h2> <div class="metadata"> <small class="text-muted" style="text-transform:uppercase;display:block;line-height:2.5em;">Conference</small><span class="authors"> <span class="author">Kruger, Albert</span> ; <span class="author">Kim, Dongsang</span> ; <span class="author">Goel, Ashutosh</span> <span class="text-muted pubdata"></span> </span> </div> <div class="abstract">A priority of the United States Department of Energy (U.S. DOE) is to dispose of nuclear wastes accumulated in 177 underground tanks at the Hanford Nuclear Reservation in eastern Washington State. These nuclear wastes date from the Manhattan Project of World War II and from plutonium production during the Cold War. The DOE plans to separate high-level radioactive wastes from low activity wastes and to treat each of the waste streams by vitrification (immobilization of the nuclides in glass) for disposal. The immobilized low-activity waste will be disposed of here at Hanford and the immobilized high-level waste at the national<a href='#' onclick='$(this).hide().next().show().next().show();return false;' style='margin-left:10px;'>more »</a><span style='display:none;'> geologic repository. Included in the inventory of highly radioactive wastes is large volumes of {sup 99}Tc (∼9 x 10 E2 TBq or ∼2.5 x 10{sup 4} Ci or ∼1500 kg). A problem facing safe disposal of Tc-bearing wastes is the processing of waste feed into in a chemically durable waste form. Technetium incorporates poorly into silicate glass in traditional glass melting. It readily evaporates during melting of glass feeds and out of the molten glass, leading to a spectrum of high-to-low retention (ca. 20 to 80%) in the cooled glass product. DOE-ORP currently has a program at Pacific Northwest National Laboratory (PNNL), in the Department of Materials Science and Engineering at Rutgers University and in the School of Mechanical and Materials Engineering at Washington State University that seeks to understand aspects of Tc retention by means of studying Tc partitioning, molten salt formation, volatilization pathways, and cold cap chemistry. Another problem involves the stability of Tc in glass in both the national geologic repository and on-site disposal after it has been immobilized. The major environmental concern with {sup 99}Tc is its high mobility in addition to a long half-life (2.1 x 10{sup 5} yrs). The pertechnetate ion (TcO{sup 4-}) is highly soluble in water and does not adsorb well onto the surface of minerals and so migrates nearly at the same velocity as groundwater. Long-term corrosion of glass waste forms is an area of current interest to the DOE, but attention to the release of Tc from glass has been little explored. It is expected that the release of Tc from glass should be highly dependent on the local glass structure as well as the chemistry of the surrounding environment, including groundwater pH. Though the speciation of Tc in glass has been previously studied, and the Tc species present in waste glass have been previously reported, environmental Tc release mechanisms are poorly understood. The recent advances in Tc chemistry that have given rise to an understanding of incorporation in the glass giving rise to significantly higher single-pass retention during vitrification are presented. Additionally, possible changes to the baseline flowsheet that allow for relatively minor volumes of Tc reporting to secondary waste treatment will be discussed. (authors)</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;"> </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; opacity: 1;"><span class="fa fa-angle-right"></span> Similar Records</a></li> </ul> </div> </div> </section> </div></div> </div> </div> </section> <footer class="" style="background-color:#f9f9f9; /* padding-top: 0.5rem; */"> <div class="footer-minor"> <div class="container"> <hr class="footer-separator" /> <div class="text-center" style="margin-top:1.25rem;"> <div class="pure-menu pure-menu-horizontal"> <ul class="pure-menu-list" id="footer-org-menu"> <li class="pure-menu-item"> <a href="https://energy.gov" target="_blank" rel="noopener noreferrer"> <img src="data:image/gif;base64,R0lGODlhAQABAIAAAP///wAAACH5BAEAAAAALAAAAAABAAEAAAICRAEAOw==" class="sprite sprite-footer-us-doe-min" alt="U.S. Department of Energy" /> </a> </li> <li class="pure-menu-item"> <a href="https://www.energy.gov/science/office-science" target="_blank" rel="noopener noreferrer"> <img src="data:image/gif;base64,R0lGODlhAQABAIAAAP///wAAACH5BAEAAAAALAAAAAABAAEAAAICRAEAOw==" class="sprite sprite-footer-office-of-science-min" alt="Office of Science" /> </a> </li> <li class="pure-menu-item"> <a href="/"> <img src="data:image/gif;base64,R0lGODlhAQABAIAAAP///wAAACH5BAEAAAAALAAAAAABAAEAAAICRAEAOw==" class="sprite sprite-footer-osti-min" alt="Office of Scientific and Technical Information" /> </a> </li> </ul> </div> </div> <div class="text-center small" style="margin-top:0.5em;margin-bottom:2.0rem;"> <div class="pure-menu pure-menu-horizontal"> <ul class="pure-menu-list"> <li class="pure-menu-item"><a href="/disclaim" class="pure-menu-link"><span class="fa fa-institution"></span> Website Policies <span class="hidden-xs">/ Important Links</span></a></li> <li class="pure-menu-item"><a href="/pages/contact" class="pure-menu-link"><span class="fa fa-comments-o"></span> Contact Us</a></li> <li class="d-block d-md-none"></li> <li class="pure-menu-item"><a href="https://www.facebook.com/ostigov" target="_blank" rel="noopener noreferrer" class="pure-menu-link social"><span class="fa fa-facebook" style=""></span></a></li> <li class="pure-menu-item"><a href="https://twitter.com/OSTIgov" target="_blank" rel="noopener noreferrer" class="pure-menu-link social"><span class="fa fa-twitter" style=""></span></a></li> <li class="pure-menu-item"><a href="https://www.youtube.com/user/ostigov" target="_blank" rel="noopener noreferrer" class="pure-menu-link social"><span class="fa fa-youtube-play" style=""></span></a></li> </ul> </div> </div> </div> </div> </footer> <link href="/pages/css/pages.fonts.210415.0019.css" rel="stylesheet"> <script src="/pages/js/pages.210415.0019.js"></script><noscript></noscript> <script defer src="/pages/js/pages.biblio.210415.0019.js"></script><noscript></noscript> <script defer src="/pages/js/lity.js"></script><noscript></noscript> <script async type="text/javascript" src="/pages/js/Universal-Federated-Analytics-Min.js?agency=DOE" id="_fed_an_ua_tag"></script><noscript></noscript> </body> <!-- DOE PAGES v.210415.0019 --> </html>