One- and Two-Electron Reductions in MiniSOG and their Implication in Catalysis
dc.contributor.author | Azpitarte Aguirre, Oxana | |
dc.contributor.author | Zudaire, Ane | |
dc.contributor.author | Uranga, Jon | |
dc.contributor.author | López de Pariza Sanz, Xabier | |
dc.contributor.author | Salassa, Luca | |
dc.contributor.author | Formoso Estensoro, Elena | |
dc.contributor.author | Rezabal Astigarraga, Elixabete | |
dc.date.accessioned | 2023-09-18T16:55:20Z | |
dc.date.available | 2023-09-18T16:55:20Z | |
dc.date.issued | 2023-08 | |
dc.identifier.citation | ChemPhysChem 24(15) : (2023) // Article ID e202300091 | es_ES |
dc.identifier.issn | 1439-4235 | |
dc.identifier.issn | 1439-7641 | |
dc.identifier.uri | http://hdl.handle.net/10810/62582 | |
dc.description.abstract | The unconventional bioorthogonal catalytic activation of anticancer metal complexes by flavin and flavoproteins photocatalysis has been reported recently. The reactivity is based on a two-electron redox reaction of the photoactivated flavin. Furthermore, when it comes to flavoproteins, we recently reported that site mutagenesis can modulate and improve this catalytic activity in the mini Singlet Oxygen Generator protein (SOG). In this paper, we analyze the reductive half-reaction in different miniSOG environments by means of density functional theory. We report that the redox properties of flavin and the resulting reactivity of miniSOG is modulated by specific mutations, which is in line with the experimental results in the literature. This modulation can be attributed to the fundamental physicochemical properties of the system, specifically (i) the competition of single and double reduction of the flavin and (ii) the probability of electron transfer from the protein to the flavin. These factors are ultimately linked to the stability of flavin‘s electron-accepting orbitals in different coordination modes. | es_ES |
dc.description.sponsorship | We acknowledge the Basque Government – Eusko Jaurlaritza (IT1254-19, IT1584-22, IkasC-2021-1-0252 (A.Z.), PIBA_2021_1_0034 (L.S.)), University of the Basque Country UPV/EHU (PIF19/244), Spanish State Research Agency (PID2019-109111RB-I00 (L.S., E.R. O.A.), PGC2018-097529-B-100 (X.L., E.F.), and FPU20/00688 (O.A.)) and Diputación Foral de Gipuzkoa (RED 2021) for financial support and the SGi/IZO-SGIker UPV/EHU for generous allocation of computational resources. Prof. Jesus Ugalde is acknowledged for fruitful discussions about electron transfer processes. L.S. thanks the Spanish Multi-MetDrugs RED2018-102471-T. This work was performed under the Severo Ochoa Centres of Excellence Programme run by the Spanish State Research Agency, CEX2018-000867-S (DIPC). | es_ES |
dc.language.iso | eng | es_ES |
dc.publisher | Wiley | es_ES |
dc.relation | info:eu-repo/grantAgreement/MICINN/PID2019-109111RB-I00 | es_ES |
dc.relation | info:eu-repo/grantAgreement/MICIU/PGC2018-097529-B-100 | es_ES |
dc.relation | info:eu-repo/grantAgreement/MICIU/CEX2018-000867-S | es_ES |
dc.rights | info:eu-repo/semantics/openAccess | es_ES |
dc.rights.uri | http://creativecommons.org/licenses/by-nc-nd/3.0/es/ | * |
dc.title | One- and Two-Electron Reductions in MiniSOG and their Implication in Catalysis | es_ES |
dc.type | info:eu-repo/semantics/article | es_ES |
dc.rights.holder | © 2023 The Authors. ChemPhysChem published by Wiley-VCH GmbH This is an open access article under the terms of the Creative Commons Attribution-NonCommercial-NoDerivs License, which permits use and distribution in any medium, provided the original work is properly cited, the use is non-commercial and no modifications or adaptations are made. | es_ES |
dc.rights.holder | Atribución-NoComercial-SinDerivadas 3.0 España | * |
dc.relation.publisherversion | https://chemistry-europe.onlinelibrary.wiley.com/doi/full/10.1002/cphc.202300091 | es_ES |
dc.identifier.doi | 10.1002/cphc.202300091 | |
dc.departamentoes | Polímeros y Materiales Avanzados: Física, Química y Tecnología | es_ES |
dc.departamentoes | Química física | es_ES |
dc.departamentoeu | Polimero eta Material Aurreratuak: Fisika, Kimika eta Teknologia | es_ES |
dc.departamentoeu | Kimika fisikoa | es_ES |
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Except where otherwise noted, this item's license is described as © 2023 The Authors. ChemPhysChem published by Wiley-VCH GmbH
This is an open access article under the terms of the Creative Commons Attribution-NonCommercial-NoDerivs License, which permits use and distribution in any medium, provided the original work is properly cited, the use is non-commercial and no modifications or adaptations are made.