Enhancement of direct electron transfer in graphene bioelectrodes containing novel cytochrome c553 variants with optimized heme orientation

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dc.authoridJacquet, Margot/0000-0002-5842-9761
dc.authoridIzzo, Miriam/0000-0003-4586-610X
dc.authoridUnlu, Cumhur Gokhan/0000-0003-2554-5886
dc.authoridKargul, Joanna/0000-0003-1410-1905
dc.authoridLasica, Anna/0000-0003-0516-9959
dc.authoridNiewiadomski, Pawel/0000-0001-6254-6162
dc.authoridOsella, Silvio/0000-0001-8541-1914
dc.contributor.authorIzzo, Miriam
dc.contributor.authorOsella, Silvio
dc.contributor.authorJacquet, Margot
dc.contributor.authorKiliszek, Malgorzata
dc.contributor.authorHarputlu, Ersan
dc.contributor.authorStarkowska, Alicja
dc.contributor.authorLasica, Anna
dc.date.accessioned2025-03-17T12:27:26Z
dc.date.available2025-03-17T12:27:26Z
dc.date.issued2021
dc.departmentTarsus Üniversitesi
dc.description.abstractThe highly efficient bioelectrodes based on single layer graphene (SLG) functionalized with pyrene self-assembled monolayer and novel cytochrome c(553) (cyt c(553)) 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 c(553) - holoprotein and the surface anchoring C-terminal His s -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 c(553) 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. (C) 2021 The Authors. Published by Elsevier B.V.
dc.description.sponsorshipPolish National Science Center [UMO-2017/27/B/ST5/00472, UMO-2018/31/D/ST4/01475]; Center of New Technologies, University of Warsaw [501-D313-86-0119600-01]
dc.description.sponsorshipMI, MK, MJ, SO and JK gratefully acknowledge the financial support from the Polish National Science Center (grants no. UMO-2017/27/B/ST5/00472 to JK and UMO-2018/31/D/ST4/01475 to SO) . MI and SO were additionally supported by Center of New Technologies, University of Warsaw (internal grant no. 501-D313-86-0119600-01 to MI and SO) .
dc.identifier.doi10.1016/j.bioelechem.2021.107818
dc.identifier.issn1567-5394
dc.identifier.issn1878-562X
dc.identifier.pmid33905959
dc.identifier.scopus2-s2.0-85104798661
dc.identifier.scopusqualityQ1
dc.identifier.urihttps://doi.org/10.1016/j.bioelechem.2021.107818
dc.identifier.urihttps://hdl.handle.net/20.500.13099/2253
dc.identifier.volume140
dc.identifier.wosWOS:000663599500010
dc.identifier.wosqualityQ1
dc.indekslendigikaynakWeb of Science
dc.indekslendigikaynakScopus
dc.indekslendigikaynakPubMed
dc.language.isoen
dc.publisherElsevier Science Sa
dc.relation.ispartofBioelectrochemistry
dc.relation.publicationcategoryMakale - Uluslararası Hakemli Dergi - Kurum Öğretim Elemanı
dc.rightsinfo:eu-repo/semantics/openAccess
dc.snmzKA_WOS_20250316
dc.subjectBiohybrid nanodevices
dc.subjectDirect electron transfer
dc.subjectCytochrome c
dc.subjectSingle layer graphene
dc.subjectQuantum mechanics/molecular mechanics
dc.titleEnhancement of direct electron transfer in graphene bioelectrodes containing novel cytochrome c553 variants with optimized heme orientation
dc.typeArticle

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