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Enhancement of Direct Electron Transfer in Graphene Bioelectrodes Containing Novel Cytochrome c Variants with Optimized Heme Orientation

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dc.abstract.enThe highly efficient bioelectrodes based on single layer graphene (SLG) functionalized with pyrene self-assembled monolayer and novel cytochrome c553 (cyt c553) peptide linker variants were rationally designed to optimize the direct electron transfer (DET) between SLG and the heme group of cyt. Through a combination of photoelectrochemical and quantum mechanical (QM/MM) approaches we show that the specific amino acid sequence of a short peptide genetically inserted between the cyt c553 holoprotein and the surface anchoring C-terminal His6-tag plays a crucial role in ensuring the optimal orientation and distance of the heme group with respect to the SLG surface. Consequently, efficient DET occurring between graphene and cyt c553 leads to a 20-fold enhancement of the cathodic photocurrent output compared to the previously reported devices of a similar type. The QM/MM modeling implies that a perpendicular or parallel orientation of the heme group with respect to the SLG surface is detrimental to DET, whereas the tilted orientation favors the cathodic photocurrent generation. Our work confirms the possibility of fine-tuning the electronic communication within complex bio-organic nanoarchitectures and interfaces due to optimization of the tilt angle of the heme group, its distance from the SLG surface and optimal HOMO/LUMO levels of the interacting redox centers.
dc.affiliationUniwersytet Warszawski
dc.contributor.authorŁasica, Anna
dc.contributor.authorUnlu, C. Gokhan
dc.contributor.authorStarkowska, Alicja
dc.contributor.authorHarputlu, Ersan
dc.contributor.authorOcakoglu, Kasim
dc.contributor.authorTrzaskowski, Bartosz
dc.contributor.authorBartosik, Dariusz
dc.contributor.authorNiewiadomski, Paweł
dc.contributor.authorOsella, Silvio
dc.contributor.authorKargul, Joanna
dc.contributor.authorJacquet, Margot
dc.contributor.authorKiliszek, Małgorzata
dc.contributor.authorIzzo, Miriam
dc.contributor.authorUśpieński, Tomasz
dc.date.accessioned2024-01-24T22:48:27Z
dc.date.available2024-01-24T22:48:27Z
dc.date.copyright2021-04-08
dc.date.issued2021
dc.description.accesstimeAT_PUBLICATION
dc.description.financePublikacja bezkosztowa
dc.description.versionORIGINAL_AUTHOR
dc.identifier.doi10.1016/J.BIOELECHEM.2021.107818
dc.identifier.issn1567-5394
dc.identifier.urihttps://repozytorium.uw.edu.pl//handle/item/106226
dc.identifier.weblinkhttps://doi.org/10.1016/j.bioelechem.2021.107818
dc.languageeng
dc.pbn.affiliationchemical sciences
dc.relation.ispartofBioelectrochemistry
dc.relation.pages107818
dc.rightsCC-BY
dc.sciencecloudnosend
dc.subject.enBiohybrid nanodevices
dc.subject.enDirect electron transfer
dc.subject.enCytochrome c
dc.subject.enSingle layer graphene
dc.subject.enQuantum Mechanics
dc.subject.enMolecular Mechanics
dc.titleEnhancement of Direct Electron Transfer in Graphene Bioelectrodes Containing Novel Cytochrome c Variants with Optimized Heme Orientation
dc.typeJournalArticle
dspace.entity.typePublication