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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.
", "funding": [ { "award": { "id": "0271asj38::13/SIRG/2137", "number": "13/SIRG/2137", "program": "SFI Starting Investigator Research Grant (SIRG)", "title": { "en": "Designing Reactive Functionalised Soft Interfaces _ Self-healing soft materials for solar energy conversion, energy storage, and sustainable low cost hydrogen production" } }, "funder": { "id": "0271asj38", "name": "Science Foundation Ireland" } }, { "award": { "acronym": "SOFT-PHOTOCONVERSION", "id": "00k4n6c32::716792", "identifiers": [ { "identifier": "https://cordis.europa.eu/projects/716792", "scheme": "url" } ], "number": "716792", "program": "H2020", "title": { "en": "Solar Energy Conversion without Solid State Architectures: Pushing the Boundaries of Photoconversion Efficiencies at Self-healing Photosensitiser Functionalised Soft Interfaces" } }, "funder": { "id": "00k4n6c32", "name": "European Commission" } } ], "publication_date": "2021-10-22", "publisher": "Zenodo", "resource_type": { "id": "publication-article", "title": { "de": "Zeitschriftenartikel", "en": "Journal article" } }, "rights": [ { "description": { "en": "The Creative Commons Attribution license allows re-distribution and re-use of a licensed work on the condition that the creator is appropriately credited." }, "icon": "cc-by-icon", "id": "cc-by-4.0", "props": { "scheme": "spdx", "url": "https://creativecommons.org/licenses/by/4.0/legalcode" }, "title": { "en": "Creative Commons Attribution 4.0 International" } } ], "subjects": [ { "subject": "sulfur oxidation" }, { "subject": "polarised liquid|liquid interface" }, { "subject": "interface between two immiscible electrolyte solutions (ITIES)" }, { "subject": "interfacial assembly" }, { "subject": "catalytic gold nanoparticles" }, { "subject": "anion physisorption" } ], "title": "Mimicking the microbial oxidation of elemental sulfur with a biphasic electrochemical cell", "version": "Published" }, "parent": { "access": { "owned_by": { "user": 201747 } }, "communities": {}, "id": "5727479", "pids": {} }, "pids": { "doi": { "identifier": "10.1016/j.electacta.2021.139443", "provider": "external" }, "oai": { "identifier": "oai:zenodo.org:5727480", "provider": "oai" } }, "revision_id": 2, "stats": { "all_versions": { "data_volume": 77521120.0, "downloads": 59, "unique_downloads": 58, "unique_views": 38, "views": 43 }, "this_version": { "data_volume": 77521120.0, "downloads": 59, "unique_downloads": 58, "unique_views": 38, "views": 43 } }, "status": "published", "updated": "2021-11-26T01:48:44.605964+00:00", "versions": { "index": 1, "is_latest": true } }