Electrochemistry of a high redox potential laccase obtained by computer-guided mutagenesis combined with directed evolution

[EN] Electrochemical characterization of the GreeDo variant of a high redox potential fungal laccase obtained by laboratory evolution together with computer-guided mutagenesis, in comparison to its parental variety (the OB-1 mutant), is presented. Both laccases, when immobilized on graphite electrod...

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Detalles Bibliográficos
Autores: Aleksejeva, Olga, Mateljak, Ivan, Ludwig, Roland, Alcalde Galeote, Miguel, Shleev, Sergey
Tipo de recurso: artículo
Estado:Versión publicada
Fecha de publicación:2019
País:España
Institución:Consejo Superior de Investigaciones Científicas (CSIC)
Repositorio:DIGITAL.CSIC. Repositorio Institucional del CSIC
OAI Identifier:oai:digital.csic.es:10261/208061
Acceso en línea:http://hdl.handle.net/10261/208061
Access Level:acceso abierto
Palabra clave:Laccase
Oxygen bioelectroreduction
Direct electron transfer
Graphite electrode
Gold nanoparticles
T1 site redox potential
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spelling Electrochemistry of a high redox potential laccase obtained by computer-guided mutagenesis combined with directed evolutionAleksejeva, OlgaMateljak, IvanLudwig, RolandAlcalde Galeote, MiguelShleev, SergeyLaccaseOxygen bioelectroreductionDirect electron transferGraphite electrodeGold nanoparticlesT1 site redox potential[EN] Electrochemical characterization of the GreeDo variant of a high redox potential fungal laccase obtained by laboratory evolution together with computer-guided mutagenesis, in comparison to its parental variety (the OB-1 mutant), is presented. Both laccases, when immobilized on graphite electrodes either by direct physical adsorption or covalently attached via gold nanoparticles, were capable of both non-mediated and mediator-based bioelectroreduction of molecular oxygen at low overpotentials. GreeDo exhibited higher open circuit potential values and onset potentials for oxygen bioelectroreduction compared to OB-1. However, even though in homogeneous catalysis GreeDo outperforms OB-1 in terms of turnover numbers and catalytic efficiency, when exposed to high redox potential substrates, direct electron transfer based bioelectrocatalytic currents of GreeDo and OB-1 modified electrodes were similar. High operational stability of freely diffusing GreeDo and also the immobilized enzyme in the acidic electrolyte was registered, in agreement with high storage stability of GreeDo in acidic solutions.The work was financially supported by the Swedish Energy Agency (P44707-1).Elsevier BVSwedish Energy AgencyConsejo Superior de Investigaciones Científicas [https://ror.org/02gfc7t72]2020202020192020info:eu-repo/semantics/articlehttp://purl.org/coar/resource_type/c_6501Publisher's versioninfo:eu-repo/semantics/publishedVersionhttp://hdl.handle.net/10261/208061reponame:DIGITAL.CSIC. Repositorio Institucional del CSICinstname:Consejo Superior de Investigaciones Científicas (CSIC)Ingléshttp://dx.doi.org/10.1016/j.elecom.2019.106511Síinfo:eu-repo/semantics/openAccessoai:digital.csic.es:10261/2080612026-05-22T06:33:51Z
dc.title.none.fl_str_mv Electrochemistry of a high redox potential laccase obtained by computer-guided mutagenesis combined with directed evolution
title Electrochemistry of a high redox potential laccase obtained by computer-guided mutagenesis combined with directed evolution
spellingShingle Electrochemistry of a high redox potential laccase obtained by computer-guided mutagenesis combined with directed evolution
Aleksejeva, Olga
Laccase
Oxygen bioelectroreduction
Direct electron transfer
Graphite electrode
Gold nanoparticles
T1 site redox potential
title_short Electrochemistry of a high redox potential laccase obtained by computer-guided mutagenesis combined with directed evolution
title_full Electrochemistry of a high redox potential laccase obtained by computer-guided mutagenesis combined with directed evolution
title_fullStr Electrochemistry of a high redox potential laccase obtained by computer-guided mutagenesis combined with directed evolution
title_full_unstemmed Electrochemistry of a high redox potential laccase obtained by computer-guided mutagenesis combined with directed evolution
title_sort Electrochemistry of a high redox potential laccase obtained by computer-guided mutagenesis combined with directed evolution
dc.creator.none.fl_str_mv Aleksejeva, Olga
Mateljak, Ivan
Ludwig, Roland
Alcalde Galeote, Miguel
Shleev, Sergey
author Aleksejeva, Olga
author_facet Aleksejeva, Olga
Mateljak, Ivan
Ludwig, Roland
Alcalde Galeote, Miguel
Shleev, Sergey
author_role author
author2 Mateljak, Ivan
Ludwig, Roland
Alcalde Galeote, Miguel
Shleev, Sergey
author2_role author
author
author
author
dc.contributor.none.fl_str_mv Swedish Energy Agency
Consejo Superior de Investigaciones Científicas [https://ror.org/02gfc7t72]
dc.subject.none.fl_str_mv Laccase
Oxygen bioelectroreduction
Direct electron transfer
Graphite electrode
Gold nanoparticles
T1 site redox potential
topic Laccase
Oxygen bioelectroreduction
Direct electron transfer
Graphite electrode
Gold nanoparticles
T1 site redox potential
description [EN] Electrochemical characterization of the GreeDo variant of a high redox potential fungal laccase obtained by laboratory evolution together with computer-guided mutagenesis, in comparison to its parental variety (the OB-1 mutant), is presented. Both laccases, when immobilized on graphite electrodes either by direct physical adsorption or covalently attached via gold nanoparticles, were capable of both non-mediated and mediator-based bioelectroreduction of molecular oxygen at low overpotentials. GreeDo exhibited higher open circuit potential values and onset potentials for oxygen bioelectroreduction compared to OB-1. However, even though in homogeneous catalysis GreeDo outperforms OB-1 in terms of turnover numbers and catalytic efficiency, when exposed to high redox potential substrates, direct electron transfer based bioelectrocatalytic currents of GreeDo and OB-1 modified electrodes were similar. High operational stability of freely diffusing GreeDo and also the immobilized enzyme in the acidic electrolyte was registered, in agreement with high storage stability of GreeDo in acidic solutions.
publishDate 2019
dc.date.none.fl_str_mv 2019
2020
2020
2020
dc.type.none.fl_str_mv info:eu-repo/semantics/article
http://purl.org/coar/resource_type/c_6501
Publisher's version
info:eu-repo/semantics/publishedVersion
format article
status_str publishedVersion
dc.identifier.none.fl_str_mv http://hdl.handle.net/10261/208061
url http://hdl.handle.net/10261/208061
dc.language.none.fl_str_mv Inglés
language_invalid_str_mv Inglés
dc.relation.none.fl_str_mv http://dx.doi.org/10.1016/j.elecom.2019.106511
Sí
dc.rights.none.fl_str_mv info:eu-repo/semantics/openAccess
eu_rights_str_mv openAccess
dc.publisher.none.fl_str_mv Elsevier BV
publisher.none.fl_str_mv Elsevier BV
dc.source.none.fl_str_mv reponame:DIGITAL.CSIC. Repositorio Institucional del CSIC
instname:Consejo Superior de Investigaciones Científicas (CSIC)
instname_str Consejo Superior de Investigaciones Científicas (CSIC)
reponame_str DIGITAL.CSIC. Repositorio Institucional del CSIC
collection DIGITAL.CSIC. Repositorio Institucional del CSIC
repository.name.fl_str_mv
repository.mail.fl_str_mv
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score 15.811543

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