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Title: Surprising formation of quasi-stable Tc( vi ) in high ionic strength alkaline media

Abstract

This work demonstrates an aqueous Tc( vi ) lifetime 6 orders of magnitude greater than previously suggested.

Authors:
ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [3]; ORCiD logo [3]; ORCiD logo [1]
  1. Energy and Environment Directorate, Pacific Northwest National Laboratory, Richland, USA
  2. Physical and Computational Sciences Directorate, Pacific Northwest National Laboratory, Richland, USA
  3. Environmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory, Richland, USA
Publication Date:
Sponsoring Org.:
USDOE
OSTI Identifier:
1438947
Grant/Contract Number:  
AC05-76RL01830
Resource Type:
Publisher's Accepted Manuscript
Journal Name:
Inorganic Chemistry Frontiers
Additional Journal Information:
Journal Name: Inorganic Chemistry Frontiers Journal Volume: 5 Journal Issue: 9; Journal ID: ISSN 2052-1553
Publisher:
Royal Society of Chemistry (RSC)
Country of Publication:
United Kingdom
Language:
English

Citation Formats

Chatterjee, Sayandev, Hall, Gabriel B., Johnson, Isaac E., Du, Yingge, Walter, Eric D., Washton, Nancy M., and Levitskaia, Tatiana G. Surprising formation of quasi-stable Tc( vi ) in high ionic strength alkaline media. United Kingdom: N. p., 2018. Web. doi:10.1039/C8QI00219C.
Chatterjee, Sayandev, Hall, Gabriel B., Johnson, Isaac E., Du, Yingge, Walter, Eric D., Washton, Nancy M., & Levitskaia, Tatiana G. Surprising formation of quasi-stable Tc( vi ) in high ionic strength alkaline media. United Kingdom. doi:10.1039/C8QI00219C.
Chatterjee, Sayandev, Hall, Gabriel B., Johnson, Isaac E., Du, Yingge, Walter, Eric D., Washton, Nancy M., and Levitskaia, Tatiana G. Mon . "Surprising formation of quasi-stable Tc( vi ) in high ionic strength alkaline media". United Kingdom. doi:10.1039/C8QI00219C.
@article{osti_1438947,
title = {Surprising formation of quasi-stable Tc( vi ) in high ionic strength alkaline media},
author = {Chatterjee, Sayandev and Hall, Gabriel B. and Johnson, Isaac E. and Du, Yingge and Walter, Eric D. and Washton, Nancy M. and Levitskaia, Tatiana G.},
abstractNote = {This work demonstrates an aqueous Tc( vi ) lifetime 6 orders of magnitude greater than previously suggested.},
doi = {10.1039/C8QI00219C},
journal = {Inorganic Chemistry Frontiers},
number = 9,
volume = 5,
place = {United Kingdom},
year = {2018},
month = {1}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
DOI: 10.1039/C8QI00219C

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Cited by: 2 works
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R.</span> </li> <li> Journal of Environment Quality, Vol. 8, Issue 2</li> <li> <span class="text-muted related-url">DOI: <a href="https://doi.org/10.2134/jeq1979.00472425000800020004x" class="text-muted" target="_blank" rel="noopener noreferrer">10.2134/jeq1979.00472425000800020004x<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/10.1039/DT9880001725" target="_blank" rel="noopener noreferrer" class="name">Preparation and crystal structures of [AsPh <sub>4</sub> ] <sub>4</sub> [Tc <sub>4</sub> N <sub>4</sub> O <sub>2</sub> (ox) <sub>6</sub> ] and [AsPh <sub>4</sub> ] <sub>2</sub> [TcO(ox) <sub>2</sub> (Hox)]·3H <sub>2</sub> O: technetium complexes containing quadridentate or unidentate oxalato ligands<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="1988-01-01">January 1988</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;"> Baldas, John; Colmanet, Silvano F.; Mackay, Maureen F.</span> </li> <li> J. Chem. Soc., Dalton Trans., Issue 7</li> <li> <span class="text-muted related-url">DOI: <a href="https://doi.org/10.1039/DT9880001725" class="text-muted" target="_blank" rel="noopener noreferrer">10.1039/DT9880001725<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/10.1039/dt9840002395" target="_blank" rel="noopener noreferrer" class="name">Studies of technetium complexes. Part 6. The preparation, characterisation, and electron spin resonance spectra of salts of tetrachloro- and tetrabromo-nitridotechnetate(VI): crystal structure of tetraphenylarsonium tetrachloronitridotechnetate(VI)<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="1984-01-01">January 1984</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;"> Baldas, John; Boas, John F.; Bonnyman, John</span> </li> <li> Journal of the Chemical Society, Dalton Transactions, Issue 11</li> <li> <span class="text-muted related-url">DOI: <a href="https://doi.org/10.1039/dt9840002395" class="text-muted" target="_blank" rel="noopener noreferrer">10.1039/dt9840002395<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/10.1016/0020-708X(82)90132-6" target="_blank" rel="noopener noreferrer" class="name">Electrochemistry of technetium<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="1982-10-01">October 1982</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;"> Russell, Charles D.</span> </li> <li> The International Journal of Applied Radiation and Isotopes, Vol. 33, Issue 10</li> <li> <span class="text-muted related-url">DOI: <a href="https://doi.org/10.1016/0020-708X(82)90132-6" class="text-muted" target="_blank" rel="noopener noreferrer">10.1016/0020-708X(82)90132-6<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="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="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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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="/pages/biblio/1501348-sequestration-vi-from-acidic-alkaline-high-ionic-strength-aqueous-media-functionalized-magnetic-mesoporous-silica-nanoparticles-capacity-binding-mechanisms" itemprop="url">Sequestration of U(VI) from Acidic, Alkaline, and High Ionic-Strength Aqueous Media by Functionalized Magnetic Mesoporous Silica Nanoparticles: Capacity and Binding Mechanisms</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">Li, Dien</span> ; <span class="author">Egodawatte, Shani</span> ; <span class="author">Kaplan, Daniel I.</span> ; <span class="author">...</span> <span class="text-muted pubdata"> - Environmental Science and Technology</span> </span> </div> <div class="abstract">Uranium(VI) exhibits little adsorption onto sediment minerals in acidic, alkaline or high ionic-strength aqueous media that often occur in U mining or contaminated sites, which makes U(VI) very mobile and difficult to sequester. In this work, magnetic mesoporous silica nanoparticles (MMSNs) were functionalized with several organic ligands. The functionalized MMSNs were highly effective and had large binding capacity for U sequestration from high salt water (HSW) simulant (54 mg U/g sorbent). The functionalized MMSNs, after U exposure in HSW simulant, pH 3.5 and 9.6 artificial groundwater (AGW), were characterized by a host of spectroscopic methods. Among the key novel findings<a href='#' onclick='$(this).hide().next().show().next().show();return false;' style='margin-left:10px;'>more »</a><span style='display:none;'> in this work was that in the HSW simulant or high pH AGW, the dominant U species bound to the functionalized MMSNs were uranyl or uranyl hydroxide, rather than uranyl carbonates as expected. The surface functional groups appear to be out-competing the carbonate ligands associated with the aqueous U species. The uranyl-like species were bound with N ligand as η<sup>2</sup> bound motifs or phosphonate ligand as a monodentate, as well as on tetrahedral Si sites as an edge-sharing bidentate. Conclusively, the N and phosphonate ligand-functionalized MMSNs hold promise as effective sorbents for sequestering U from acidic, alkaline or high ionic-strength contaminated aqueous media.</span><a href='#' onclick='$(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 9<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.7b03778" target="_blank" rel="noopener" title="Link to document DOI" data-ostiid="1501348" data-product-type="Journal Article" data-product-subtype="AM" >10.1021/acs.est.7b03778</a></span></li> <li class="pure-menu-item"><span class="item-info-ftlink"><a class="misc fulltext-link " href="/pages/servlets/purl/1501348" title="Link to document media" target="_blank" rel="noopener" data-ostiid="1501348" 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="1" /><div class="item-info"> <h2 class="title" itemprop="name headline"><a href="/biblio/1612056-actinyl-cation-interactions-experimental-theoretical-assessment-np-vi-cl-vi-cl-systems" itemprop="url">Actinyl-cation interactions: experimental and theoretical assessment of [Np( vi )O <sub>2</sub> Cl <sub>4</sub> ] <sup>2-</sup> and [U( vi )O <sub>2</sub> Cl <sub>4</sub> ] <sup>2-</sup> systems</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">Bjorklund, Jennifer L.</span> ; 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<span class="author">Klepov, Vladislav V.</span> ; <span class="author">Morrison, Gregory</span> ; <span class="author">...</span> <span class="text-muted pubdata"> - ChemComm</span> </span> </div> <div class="abstract">The synthesis of five new U( iv , v ) and U( v , vi ) silicates points toward moderate supercritical synthesis as a new route to the stabilization of mixed-valent uranium compounds.</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 1<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/C8CC07789D" target="_blank" rel="noopener" title="Link to document DOI" data-ostiid="1479120" data-product-type="Journal Article" data-product-subtype="PM" >10.1039/C8CC07789D</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/1566628-moderate-supercritical-synthesis-facile-route-mixed-valent-uranium-iv-vi-silicates" itemprop="url">Moderate supercritical synthesis as a facile route to mixed-valent uranium( iv , v ) and ( v , vi ) silicates</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">Pace, Kristen A.</span> ; 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