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Diazonium-Based Covalent Molecular Wiring of Single-Layer Graphene Leads to Enhanced Unidirectional Photocurrent Generation through the p-doping Effect

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cris.lastimport.scopus2024-02-12T19:48:36Z
dc.abstract.enDevelopment of robust and cost-effective smart materials requires rational chemical nanoengineering to provide viable technological solutions for a wide range of applications. Recently, a powerful approach based on the electrografting of diazonium salts has attracted a great deal of attention due to its numerous technological advantages. Several studies on graphene-based materials reveal that the covalent attachment of aryl groups via the above approach could lead to additional beneficial properties of this versatile material. Here, we developed the covalently linked metalorganic wires on two transparent, cheap, and conductive materials: fluorine-doped tin oxide (FTO) and FTO/single-layer graphene (FTO/SLG). The wires are terminated with nitrilotriacetic acid metal complexes, which are universal molecular anchors to immobilize His6-tagged proteins, such as biophotocatalysts and other types of redox-active proteins of great interest in biotechnology, optoelectronics, and artificial photosynthesis. We show for the first time that the covalent grafting of a diazonium salt precursor on two different electron-rich surfaces leads to the formation of the molecular wires that promote p-doping of SLG concomitantly with a significantly enhanced unidirectional cathodic photocurrent up to 1 μA cm–2. Density functional theory modeling reveals that the exceptionally high photocurrent values are due to two distinct mechanisms of electron transfer originating from different orbitals/bands of the diazonium-derived wires depending on the nature of the chelating metal redox center. Importantly, the novel metalorganic interfaces reported here exhibit minimized back electron transfer, which is essential for the maximization of solar conversion efficiency.
dc.affiliationUniwersytet Warszawski
dc.contributor.authorWięckowska, Agnieszka
dc.contributor.authorPałys, Barbara
dc.contributor.authorKargul, Joanna
dc.contributor.authorKazimierczuk, Krzysztof
dc.contributor.authorTrzaskowski, Bartosz
dc.contributor.authorKałek, Marcin
dc.contributor.authorOsella, Silvio
dc.contributor.authorJacquet, Margot
dc.contributor.authorPisarek, Marcin
dc.contributor.authorLisowski, Wojciech
dc.contributor.authorMichałowski, Paweł
dc.contributor.authorOcakoglu, Kasim
dc.contributor.authorUnlu, C. Gokhan
dc.contributor.authorRajkiewicz, Adam A.
dc.contributor.authorNawrocka, Ewa K.
dc.contributor.authorKaczmarek, Monika
dc.contributor.authorHarputlu, Ersan
dc.date.accessioned2024-01-24T21:48:22Z
dc.date.available2024-01-24T21:48:22Z
dc.date.copyright2022-04-12
dc.date.issued2022
dc.description.accesstimeAT_PUBLICATION
dc.description.financePublikacja bezkosztowa
dc.description.number8
dc.description.versionFINAL_PUBLISHED
dc.description.volume34
dc.identifier.doi10.1021/ACS.CHEMMATER.2C00088
dc.identifier.issn0897-4756
dc.identifier.urihttps://repozytorium.uw.edu.pl//handle/item/104809
dc.identifier.weblinkhttps://pubs.acs.org/doi/pdf/10.1021/acs.chemmater.2c00088
dc.languageeng
dc.pbn.affiliationchemical sciences
dc.relation.ispartofChemistry of Materials
dc.relation.pages3744-3758
dc.rightsCC-BY
dc.sciencecloudnosend
dc.titleDiazonium-Based Covalent Molecular Wiring of Single-Layer Graphene Leads to Enhanced Unidirectional Photocurrent Generation through the p-doping Effect
dc.typeJournalArticle
dspace.entity.typePublication