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

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dc.contributor.author Molina-Osorio, Andrés F.
dc.contributor.author Cheung, David L.
dc.contributor.author O'Dwyer, Colm
dc.contributor.author Stewart, Andrew A.
dc.contributor.author Dossot, Manuel
dc.contributor.author Herzog, Grégoire
dc.contributor.author Scanlon, Micheál D.
dc.date.accessioned 2020-03-11T12:46:45Z
dc.date.available 2020-03-11T12:46:45Z
dc.date.issued 2020-03-06
dc.identifier.citation Molina-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.0c00437 en
dc.identifier.startpage 1 en
dc.identifier.endpage 34 en
dc.identifier.issn 1932-7447
dc.identifier.uri http://hdl.handle.net/10468/9754
dc.identifier.doi 10.1021/acs.jpcc.0c00437 en
dc.description.abstract One 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.sponsorship Irish 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.format.mimetype application/pdf en
dc.language.iso en en
dc.publisher American Chemical Society en
dc.relation.uri https://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.0c00437 en
dc.subject Nanostructures en
dc.subject Porphyrins en
dc.subject Self-assembly en
dc.subject Light-harvesting antennas en
dc.subject Artificial photosynthesis technologies en
dc.subject Energy conversion en
dc.title Self-assembly of porphyrin nanostructures at the interface between two immiscible liquids en
dc.type Article (peer-reviewed) en
dc.internal.authorcontactother Colm O'Dwyer, Chemistry, University College Cork, Cork, Ireland. +353-21-490-3000 Email: c.odwyer@ucc.ie en
dc.internal.availability Full text available en
dc.check.info Access to this article is restricted until 12 months after publication by request of the publisher. en
dc.check.date 2021-03-06
dc.date.updated 2020-03-11T12:32:03Z
dc.description.version Accepted Version en
dc.internal.rssid 505828050
dc.contributor.funder European Research Council en
dc.contributor.funder Science Foundation Ireland en
dc.contributor.funder Campus France en
dc.contributor.funder Université de Lorraine en
dc.description.status Peer reviewed en
dc.identifier.journaltitle The Journal of Physical Chemistry C en
dc.internal.copyrightchecked Yes
dc.internal.licenseacceptance Yes en
dc.internal.IRISemailaddress c.odwyer@ucc.ie en
dc.internal.bibliocheck In press. Check vol / issue / page range. Amend citation as necessary. en
dc.relation.project info: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-PHOTOCONVERSION en
dc.relation.project info: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


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