Journal article Open Access

Mimicking the microbial oxidation of elemental sulfur with a biphasic electrochemical cell

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


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    <subfield code="a">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.</subfield>
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    <subfield code="a">Suárez-Herrera, Marco F.</subfield>
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    <subfield code="a">Mimicking the microbial oxidation of elemental sulfur with a biphasic electrochemical cell</subfield>
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    <subfield code="a">&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;</subfield>
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    <subfield code="a">10.1016/j.electacta.2021.139443</subfield>
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