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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    "title": "Mimicking the microbial oxidation of elemental sulfur with a biphasic electrochemical cell", 
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    "keywords": [
      "sulfur oxidation", 
      "polarised liquid|liquid interface", 
      "interface between two immiscible electrolyte solutions (ITIES)", 
      "interfacial assembly", 
      "catalytic gold nanoparticles", 
      "anion physisorption"
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    "publication_date": "2021-10-22", 
    "creators": [
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        "orcid": "0000-0002-7624-5982", 
        "affiliation": "Departamento De Qu\u00edmica, Facultad De Ciencias, Universidad Nacional De Colombia, Cra 30 # 45-03, Edificio 451, Bogot\u00e1, Colombia", 
        "name": "Su\u00e1rez-Herrera, Marco F."
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        "orcid": "0000-0002-7173-2861", 
        "affiliation": "The Bernal Institute and Department of Chemical Sciences, School of Natural Sciences, University of Limerick (UL), Limerick V94 T9PX, Ireland", 
        "name": "Gamero-Quijano, Alonso"
      }, 
      {
        "orcid": "0000-0002-9570-8110", 
        "affiliation": "Instituto de Electroqu\u00edmica, Universidad de Alicante, Ap.99, E\u201303080, Alicante, Spain", 
        "name": "Solla-Gull\u00f3n, Jos\u00e9"
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        "orcid": "0000-0001-7951-7085", 
        "affiliation": "The Bernal Institute and Department of Chemical Sciences, School of Natural Sciences, University of Limerick (UL), Limerick V94 T9PX, Ireland", 
        "name": "Scanlon, Miche\u00e1l D."
      }
    ], 
    "notes": "M.F.S.-H. acknowledges the \"Universidad Nacional de Colombia\" for allowing his sabbatical leave and the \"Fundaci\u00f3n Banco de la Rep\u00fablica\" through the grant 4.562.", 
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    "description": "<p>The lack of an artificial system that mimics elemental sulfur (S<sub>8</sub>) 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<sub>8</sub>, overcoming the incompatible solubilities of the hydrophobic reactants (O<sub>2</sub> and S<sub>8</sub>) and hydrophilic products (H<sup>+</sup>, SO<sub>3</sub><sup>2&ndash;</sup>, SO<sub>4</sub><sup>2&ndash;</sup>, <em>etc.</em>). Furthermore, the interfacial AuNPs provide a catalytic surface onto which O<sub>2</sub> and S<sub>8</sub> 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<sub>2</sub>, gold and S<sub>8</sub> in biphasic systems.</p>"
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