10.1016/j.electacta.2021.139443
https://zenodo.org/records/5727480
oai:zenodo.org:5727480
Suárez-Herrera, Marco F.
Marco F.
Suárez-Herrera
0000-0002-7624-5982
Departamento De Química, Facultad De Ciencias, Universidad Nacional De Colombia, Cra 30 # 45-03, Edificio 451, Bogotá, Colombia
Gamero-Quijano, Alonso
Alonso
Gamero-Quijano
0000-0002-7173-2861
The Bernal Institute and Department of Chemical Sciences, School of Natural Sciences, University of Limerick (UL), Limerick V94 T9PX, Ireland
Solla-Gullón, José
José
Solla-Gullón
0000-0002-9570-8110
Instituto de Electroquímica, Universidad de Alicante, Ap.99, E–03080, Alicante, Spain
Scanlon, Micheál D.
Micheál D.
Scanlon
0000-0001-7951-7085
The Bernal Institute and Department of Chemical Sciences, School of Natural Sciences, University of Limerick (UL), Limerick V94 T9PX, Ireland
Mimicking the microbial oxidation of elemental sulfur with a biphasic electrochemical cell
Zenodo
2021
sulfur oxidation
polarised liquid|liquid interface
interface between two immiscible electrolyte solutions (ITIES)
interfacial assembly
catalytic gold nanoparticles
anion physisorption
2021-10-22
Published
Creative Commons Attribution 4.0 International
The lack of an artificial system that mimics elemental sulfur (S8) 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 S8, overcoming the incompatible solubilities of the hydrophobic reactants (O2 and S8) and hydrophilic products (H+, SO32–, SO42–, etc.). Furthermore, the interfacial AuNPs provide a catalytic surface onto which O2 and S8 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 O2, gold and S8 in biphasic systems.
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.
Science Foundation Ireland
10.13039/501100001602
13/SIRG/2137
Designing Reactive Functionalised Soft Interfaces _ Self-healing soft materials for solar energy conversion, energy storage, and sustainable low cost hydrogen production
European Commission
10.13039/501100000780
716792
Solar Energy Conversion without Solid State Architectures: Pushing the Boundaries of Photoconversion Efficiencies at Self-healing Photosensitiser Functionalised Soft Interfaces