October 22, 2021 Journal article Open Access

Suárez-Herrera, Marco F.; Gamero-Quijano, Alonso; Solla-Gullón, José; Scanlon, Micheál D.

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        <foaf:name>Suárez-Herrera, Marco F.</foaf:name>
        <foaf:givenName>Marco F.</foaf:givenName>
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            <foaf:name>Departamento De Química, Facultad De Ciencias, Universidad Nacional De Colombia, Cra 30 # 45-03, Edificio 451, Bogotá, Colombia</foaf:name>
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        <foaf:name>Gamero-Quijano, Alonso</foaf:name>
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            <foaf:name>The Bernal Institute and Department of Chemical Sciences, School of Natural Sciences, University of Limerick (UL), Limerick V94 T9PX, Ireland</foaf:name>
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        <foaf:name>Solla-Gullón, José</foaf:name>
        <foaf:givenName>José</foaf:givenName>
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            <foaf:name>Instituto de Electroquímica, Universidad de Alicante, Ap.99, E–03080, Alicante, Spain</foaf:name>
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        <foaf:name>Scanlon, Micheál D.</foaf:name>
        <foaf:givenName>Micheál D.</foaf:givenName>
        <foaf:familyName>Scanlon</foaf:familyName>
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            <foaf:name>The Bernal Institute and Department of Chemical Sciences, School of Natural Sciences, University of Limerick (UL), Limerick V94 T9PX, Ireland</foaf:name>
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    <dct:title>Mimicking the microbial oxidation of elemental sulfur with a biphasic electrochemical cell</dct:title>
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    <dct:issued rdf:datatype="http://www.w3.org/2001/XMLSchema#gYear">2021</dct:issued>
    <dcat:keyword>sulfur oxidation</dcat:keyword>
    <dcat:keyword>polarised liquid|liquid interface</dcat:keyword>
    <dcat:keyword>interface between two immiscible electrolyte solutions (ITIES)</dcat:keyword>
    <dcat:keyword>interfacial assembly</dcat:keyword>
    <dcat:keyword>catalytic gold nanoparticles</dcat:keyword>
    <dcat:keyword>anion physisorption</dcat:keyword>
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        <dct:identifier rdf:datatype="http://www.w3.org/2001/XMLSchema#string">10.13039/100010661</dct:identifier>
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    <dct:description>&lt;p&gt;The lack of an artificial system that mimics elemental sulfur (S&lt;sub&gt;8&lt;/sub&gt;) oxidation by microorganisms inhibits a deep mechanistic understanding of the sulfur cycle in the biosphere and the metabolism of sulfur-oxidising microorganisms. In this article, we present a biphasic system that mimics biochemical sulfur oxidation under ambient conditions using a liquid|liquid (L|L) electrochemical cell and gold nanoparticles (AuNPs) as an interfacial catalyst. The interface between two solvents of very different polarity is an ideal environment to oxidise S&lt;sub&gt;8&lt;/sub&gt;, overcoming the incompatible solubilities of the hydrophobic reactants (O&lt;sub&gt;2&lt;/sub&gt; and S&lt;sub&gt;8&lt;/sub&gt;) and hydrophilic products (H&lt;sup&gt;+&lt;/sup&gt;, SO&lt;sub&gt;3&lt;/sub&gt;&lt;sup&gt;2&amp;ndash;&lt;/sup&gt;, SO&lt;sub&gt;4&lt;/sub&gt;&lt;sup&gt;2&amp;ndash;&lt;/sup&gt;, &lt;em&gt;etc.&lt;/em&gt;). Furthermore, the interfacial AuNPs provide a catalytic surface onto which O&lt;sub&gt;2&lt;/sub&gt; and S&lt;sub&gt;8&lt;/sub&gt; can adsorb. Control over the driving force for the reaction is provided by polarising the L|L interface externally and tuning the Fermi level of the interfacial AuNPs by the adsorption of aqueous anions. Comparison of electrochemical measurements using a 4-electrode closed bipolar electrochemical cell and a L|L electrochemical cell confirmed that electron transfer reactions are possible between O&lt;sub&gt;2&lt;/sub&gt;, gold and S&lt;sub&gt;8&lt;/sub&gt; in biphasic systems.&lt;/p&gt;</dct:description>
    <dct:description>M.F.S.-H. acknowledges the "Universidad Nacional de Colombia" for allowing his sabbatical leave and the "Fundación Banco de la República" through the grant 4.562.</dct:description>
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