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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    <subfield code="a">&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;</subfield>
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    <subfield code="a">Temperature‒dependent luminescence spectroscopic and mass spectrometric investigations of U(VI) complexation with aqueous silicates in the acidic pH‒range</subfield>
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