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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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  <identifier identifierType="URL">https://zenodo.org/record/5727480</identifier>
  <creators>
    <creator>
      <creatorName>Suárez-Herrera, Marco F.</creatorName>
      <givenName>Marco F.</givenName>
      <familyName>Suárez-Herrera</familyName>
      <nameIdentifier nameIdentifierScheme="ORCID" schemeURI="http://orcid.org/">0000-0002-7624-5982</nameIdentifier>
      <affiliation>Departamento De Química, Facultad De Ciencias, Universidad Nacional De Colombia, Cra 30 # 45-03, Edificio 451, Bogotá, Colombia</affiliation>
    </creator>
    <creator>
      <creatorName>Gamero-Quijano, Alonso</creatorName>
      <givenName>Alonso</givenName>
      <familyName>Gamero-Quijano</familyName>
      <nameIdentifier nameIdentifierScheme="ORCID" schemeURI="http://orcid.org/">0000-0002-7173-2861</nameIdentifier>
      <affiliation>The Bernal Institute and Department of Chemical Sciences, School of Natural Sciences, University of Limerick (UL), Limerick V94 T9PX, Ireland</affiliation>
    </creator>
    <creator>
      <creatorName>Solla-Gullón, José</creatorName>
      <givenName>José</givenName>
      <familyName>Solla-Gullón</familyName>
      <nameIdentifier nameIdentifierScheme="ORCID" schemeURI="http://orcid.org/">0000-0002-9570-8110</nameIdentifier>
      <affiliation>Instituto de Electroquímica, Universidad de Alicante, Ap.99, E–03080, Alicante, Spain</affiliation>
    </creator>
    <creator>
      <creatorName>Scanlon, Micheál D.</creatorName>
      <givenName>Micheál D.</givenName>
      <familyName>Scanlon</familyName>
      <nameIdentifier nameIdentifierScheme="ORCID" schemeURI="http://orcid.org/">0000-0001-7951-7085</nameIdentifier>
      <affiliation>The Bernal Institute and Department of Chemical Sciences, School of Natural Sciences, University of Limerick (UL), Limerick V94 T9PX, Ireland</affiliation>
    </creator>
  </creators>
  <titles>
    <title>Mimicking the microbial oxidation of elemental sulfur with a biphasic electrochemical cell</title>
  </titles>
  <publisher>Zenodo</publisher>
  <publicationYear>2021</publicationYear>
  <subjects>
    <subject>sulfur oxidation</subject>
    <subject>polarised liquid|liquid interface</subject>
    <subject>interface between two immiscible electrolyte solutions (ITIES)</subject>
    <subject>interfacial assembly</subject>
    <subject>catalytic gold nanoparticles</subject>
    <subject>anion physisorption</subject>
  </subjects>
  <dates>
    <date dateType="Issued">2021-10-22</date>
  </dates>
  <resourceType resourceTypeGeneral="JournalArticle"/>
  <alternateIdentifiers>
    <alternateIdentifier alternateIdentifierType="url">https://zenodo.org/record/5727480</alternateIdentifier>
  </alternateIdentifiers>
  <relatedIdentifiers>
    <relatedIdentifier relatedIdentifierType="DOI" relationType="IsIdenticalTo">10.1016/j.electacta.2021.139443</relatedIdentifier>
  </relatedIdentifiers>
  <version>Published</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;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;</description>
    <description descriptionType="Other">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.</description>
  </descriptions>
  <fundingReferences>
    <fundingReference>
      <funderName>Science Foundation Ireland</funderName>
      <funderIdentifier funderIdentifierType="Crossref Funder ID">10.13039/501100001602</funderIdentifier>
      <awardNumber awardURI="info:eu-repo/grantAgreement/SFI/SFI+Starting+Investigator+Research+Grant+%28SIRG%29/13%2FSIRG%2F2137/">13/SIRG/2137</awardNumber>
      <awardTitle>Designing Reactive Functionalised Soft Interfaces _ Self-healing soft materials for solar energy conversion, energy storage, and sustainable low cost hydrogen production</awardTitle>
    </fundingReference>
    <fundingReference>
      <funderName>European Commission</funderName>
      <funderIdentifier funderIdentifierType="Crossref Funder ID">10.13039/100010661</funderIdentifier>
      <awardNumber awardURI="info:eu-repo/grantAgreement/EC/H2020/716792/">716792</awardNumber>
      <awardTitle>Solar Energy Conversion without Solid State Architectures: Pushing the Boundaries of Photoconversion Efficiencies at Self-healing Photosensitiser Functionalised Soft Interfaces</awardTitle>
    </fundingReference>
  </fundingReferences>
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