January 6, 2020 Dataset Open Access

Lösch, Henry; Raiwa, Manuel; Jordan, Norbert; Steppert, Michael; Steudtner, Robin; Stumpf, Thorsten; Huittinen, Nina Maria

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  <identifier identifierType="DOI">10.14278/rodare.211</identifier>
  <creators>
    <creator>
      <creatorName>Lösch, Henry</creatorName>
      <givenName>Henry</givenName>
      <familyName>Lösch</familyName>
      <affiliation>HZDR</affiliation>
    </creator>
    <creator>
      <creatorName>Raiwa, Manuel</creatorName>
      <givenName>Manuel</givenName>
      <familyName>Raiwa</familyName>
      <affiliation>Institute of Radioecology and Radiation Protection, Leibniz Universität Hannover</affiliation>
    </creator>
    <creator>
      <creatorName>Jordan, Norbert</creatorName>
      <givenName>Norbert</givenName>
      <familyName>Jordan</familyName>
      <nameIdentifier nameIdentifierScheme="ORCID" schemeURI="http://orcid.org/">0000-0002-4625-1580</nameIdentifier>
      <affiliation>HZDR</affiliation>
    </creator>
    <creator>
      <creatorName>Steppert, Michael</creatorName>
      <givenName>Michael</givenName>
      <familyName>Steppert</familyName>
      <affiliation>Institute of Radioecology and Radiation Protection, Leibniz Universität Hannover</affiliation>
    </creator>
    <creator>
      <creatorName>Steudtner, Robin</creatorName>
      <givenName>Robin</givenName>
      <familyName>Steudtner</familyName>
      <affiliation>HZDR</affiliation>
    </creator>
    <creator>
      <creatorName>Stumpf, Thorsten</creatorName>
      <givenName>Thorsten</givenName>
      <familyName>Stumpf</familyName>
      <affiliation>HZDR</affiliation>
    </creator>
    <creator>
      <creatorName>Huittinen, Nina Maria</creatorName>
      <givenName>Nina Maria</givenName>
      <familyName>Huittinen</familyName>
      <affiliation>HZDR</affiliation>
    </creator>
  </creators>
  <titles>
    <title>Temperature‒dependent luminescence spectroscopic and mass spectrometric investigations of U(VI) complexation with aqueous silicates in the acidic pH‒range</title>
  </titles>
  <publisher>Rodare</publisher>
  <publicationYear>2020</publicationYear>
  <subjects>
    <subject>luminescence</subject>
    <subject>silicates</subject>
    <subject>Uranium(VI)</subject>
    <subject>complexation</subject>
    <subject>thermodynamic constants</subject>
    <subject>temperature dependent</subject>
  </subjects>
  <dates>
    <date dateType="Issued">2020-01-06</date>
  </dates>
  <language>en</language>
  <resourceType resourceTypeGeneral="Dataset"/>
  <alternateIdentifiers>
    <alternateIdentifier alternateIdentifierType="url">https://rodare.hzdr.de/record/211</alternateIdentifier>
  </alternateIdentifiers>
  <relatedIdentifiers>
    <relatedIdentifier relatedIdentifierType="URL" relationType="IsIdenticalTo">https://www.hzdr.de/publications/Publ-29643</relatedIdentifier>
    <relatedIdentifier relatedIdentifierType="DOI" relationType="IsVersionOf">10.14278/rodare.210</relatedIdentifier>
    <relatedIdentifier relatedIdentifierType="URL" relationType="IsPartOf">https://rodare.hzdr.de/communities/rodare</relatedIdentifier>
  </relatedIdentifiers>
  <version>Version_1_2020-01-06</version>
  <rightsList>
    <rights rightsURI="https://creativecommons.org/licenses/by/4.0/legalcode">Creative Commons Attribution 4.0 International</rights>
    <rights rightsURI="info:eu-repo/semantics/openAccess">Open Access</rights>
  </rightsList>
  <descriptions>
    <description descriptionType="Abstract">&lt;p&gt;In this study the complexation of U(VI) with orthosilicic acid (H&lt;sub&gt;4&lt;/sub&gt;SiO&lt;sub&gt;4&lt;/sub&gt;) between pH 3.5 and 5 with electrospray ionization mass spectrometry (ESI‒MS) and laser‒induced luminescence spectroscopy was comprehensively characterized. The ESI‒MS experiments performed at a total silicon concentration of 5∙10&lt;sup&gt;‒5&lt;/sup&gt; M (exceeding the solubility of amorphous silica at both pH‒values) revealed the formation of oligomeric sodium‒silicates in addition to the UO&lt;sub&gt;2&lt;/sub&gt;OSi(OH)&lt;sub&gt;3&lt;/sub&gt;&lt;sup&gt;+&lt;/sup&gt; species. For the luminescence spectroscopic experiments (25 &amp;deg;C), the U(VI) concentration was fixed at 5∙10&lt;sup&gt;‒6&lt;/sup&gt; M, the silicon concentration was varied between 1.3∙10&lt;sup&gt;‒4&lt;/sup&gt; ‒ 1.3∙10&lt;sup&gt;‒3&lt;/sup&gt; M (reducing the formation of silicon oligomers) and the ionic strength was kept constant at 0.2 M NaClO&lt;sub&gt;4&lt;/sub&gt;. The results confirmed the formation of the aqueous UO&lt;sub&gt;2&lt;/sub&gt;OSi(OH)&lt;sub&gt;3&lt;/sub&gt;&lt;sup&gt;+&lt;/sup&gt; complex. The conditional complexation constant at 25 &amp;deg;C, log *&amp;beta; = ‒0.31&amp;plusmn; 0.24, was extrapolated to infinite dilution using the Davies equation, which led to log *&amp;beta;&lt;sup&gt;0&lt;/sup&gt; = ‒0.06 &amp;plusmn; 0.24. Further experiments at different temperatures (1 &amp;ndash; 25 &amp;deg;C) allowed the calculation of the molal enthalpy of reaction &amp;Delta;&lt;sub&gt;r&lt;/sub&gt;H&lt;sub&gt;m&lt;/sub&gt;&lt;sup&gt;0&lt;/sup&gt; = 45.8 &amp;plusmn; 22.5 kJ∙mol‒1 and molal entropy of reaction &amp;Delta;&lt;sub&gt;r&lt;/sub&gt;S&lt;sub&gt;m&lt;/sub&gt;&lt;sup&gt;0&lt;/sup&gt; = 152.5 &amp;plusmn; 78.8 J∙K‒1∙mol‒1 using the van&amp;rsquo;t Hoff equation, corroborating an endothermic and entropy driven complexation process.&lt;/p&gt;</description>
  </descriptions>
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