Self-assembly of porphyrin nanostructures at the interface between two immiscible liquids

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dc.contributor.authorMolina-Osorio, Andrés F.
dc.contributor.authorCheung, David L.
dc.contributor.authorO'Dwyer, Colm
dc.contributor.authorStewart, Andrew A.
dc.contributor.authorDossot, Manuel
dc.contributor.authorHerzog, Grégoire
dc.contributor.authorScanlon, Micheál D.
dc.contributor.funderEuropean Research Councilen
dc.contributor.funderScience Foundation Irelanden
dc.contributor.funderCampus Franceen
dc.contributor.funderUniversité de Lorraineen
dc.date.accessioned2020-03-11T12:46:45Z
dc.date.available2020-03-11T12:46:45Z
dc.date.issued2020-03-06
dc.date.updated2020-03-11T12:32:03Z
dc.description.abstractOne of the many evolved functions of photosynthetic organisms is to synthesize light harvesting nanostructures from photoactive molecules such as porphyrins. Engineering synthetic analogues with optimized molecular order necessary for the efficient capture and harvest of light energy remains challenging. Here, we address this challenge by reporting the self-assembly of zinc(II) meso-tetrakis(4-carboxyphenyl)porphyrins into films of highly ordered nanostructures. The self-assembly process takes place selectively at the interface between two immiscible liquids (water|organic solvent), with kinetically stable interfacial nanostructures formed only at pH values close to the pKa of the carboxyphenyl groups. Molecular dynamics simulations suggest that the assembly process is driven by an interplay between the hydrophobicity gradient at the interface and hydrogen bonding in the formed nanostructure. Ex situ XRD analysis and in situ UV/vis and steady state fluorescence indicates the formation of chlathrate type nanostructures that retain the emission properties of their monomeric constituents. The self-assembly method presented here avoids the use of acidic conditions, additives such as surfactants and external stimuli, offering an alternative for the realization of light-harvesting antennas in artificial photosynthesis technologies.en
dc.description.sponsorshipIrish Research Council (New Foundations Awards (2014 and 2015)); Science Foundation Ireland and Campus France (joint ULYSSES programme); Investissement d’Avenir ((PIA) “Lorraine Université d’Excellence” (Reference No. ANR-15- IDEX-04-LUE))en
dc.description.statusPeer revieweden
dc.description.versionAccepted Versionen
dc.format.mimetypeapplication/pdfen
dc.identifier.citationMolina-Osorio, A. F., Cheung, D. L., O'Dwyer, C., Stewart, A. A., Dossot, M., Herzog, G. and Scanlon, M. D. (2020) 'Self-Assembly of Porphyrin Nanostructures at the Interface Between Two Immiscible Liquids', The Journal of Physical Chemistry C, doi: 10.1021/acs.jpcc.0c00437en
dc.identifier.doi10.1021/acs.jpcc.0c00437en
dc.identifier.endpage34en
dc.identifier.issn1932-7447
dc.identifier.journaltitleThe Journal of Physical Chemistry Cen
dc.identifier.startpage1en
dc.identifier.urihttps://hdl.handle.net/10468/9754
dc.language.isoenen
dc.publisherAmerican Chemical Societyen
dc.relation.projectinfo:eu-repo/grantAgreement/EC/H2020::ERC::ERC-STG/716792/EU/Solar Energy Conversion without Solid State Architectures: Pushing the Boundaries of Photoconversion Efficiencies at Self-healing Photosensitiser Functionalised Soft Interfaces/SOFT-PHOTOCONVERSIONen
dc.relation.projectinfo:eu-repo/grantAgreement/SFI/SFI Starting Investigator Research Grant (SIRG)/13/SIRG/2137/IE/Designing Reactive Functionalised Soft Interfaces _ Self-healing soft materials for solar energy conversion, energy storage, and sustainable low cost hydrogen production/en
dc.relation.urihttps://pubs.acs.org/doi/10.1021/acs.jpcc.0c00437
dc.rights© 2020 American Chemical Society. This document is the Accepted Manuscript version of a Published Work that appeared in final form in The Journal of Physical Chemistry C, copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see https://pubs.acs.org/doi/10.1021/acs.jpcc.0c00437en
dc.subjectNanostructuresen
dc.subjectPorphyrinsen
dc.subjectSelf-assemblyen
dc.subjectLight-harvesting antennasen
dc.subjectArtificial photosynthesis technologiesen
dc.subjectEnergy conversionen
dc.titleSelf-assembly of porphyrin nanostructures at the interface between two immiscible liquidsen
dc.typeArticle (peer-reviewed)en
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