Reversible and Selective Interconversion of Hydrogen and Carbon Dioxide into Formate by a Semiartificial Formate Hydrogenlyase Mimic

Detalhes bibliográficos
Autor(a) principal: Sokol, Katarzyna P.
Data de Publicação: 2019
Outros Autores: Robinson, William E., Oliveira, Ana R., Zacarias, Sonia, Lee, Chong Yong, Madden, Christopher, Bassegoda, Arnau, Hirst, Judy, Pereira, Inês A.C., Reisner, Erwin
Tipo de documento: Artigo
Idioma: eng
Título da fonte: Repositório Científico de Acesso Aberto de Portugal (Repositórios Cientìficos)
Texto Completo: http://hdl.handle.net/10362/91347
Resumo: The biological formate hydrogenlyase (FHL) complex links a formate dehydrogenase (FDH) to a hydrogenase (H2ase) and produces H2 and CO2 from formate via mixed-acid fermentation in Escherichia coli. Here, we describe an electrochemical and a colloidal semiartificial FHL system that consists of an FDH and a H2ase immobilized on conductive indium tin oxide (ITO) as an electron relay. These in vitro systems benefit from the efficient wiring of a highly active enzyme pair and allow for the reversible conversion of formate to H2 and CO2 under ambient temperature and pressure. The hybrid systems provide a template for the design of synthetic catalysts and surpass the FHL complex in vivo by storing and releasing H2 on demand by interconverting CO2/H2 and formate with minimal bias in either direction.
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spelling Reversible and Selective Interconversion of Hydrogen and Carbon Dioxide into Formate by a Semiartificial Formate Hydrogenlyase MimicCatalysisChemistry(all)BiochemistryColloid and Surface ChemistryThe biological formate hydrogenlyase (FHL) complex links a formate dehydrogenase (FDH) to a hydrogenase (H2ase) and produces H2 and CO2 from formate via mixed-acid fermentation in Escherichia coli. Here, we describe an electrochemical and a colloidal semiartificial FHL system that consists of an FDH and a H2ase immobilized on conductive indium tin oxide (ITO) as an electron relay. These in vitro systems benefit from the efficient wiring of a highly active enzyme pair and allow for the reversible conversion of formate to H2 and CO2 under ambient temperature and pressure. The hybrid systems provide a template for the design of synthetic catalysts and surpass the FHL complex in vivo by storing and releasing H2 on demand by interconverting CO2/H2 and formate with minimal bias in either direction.Instituto de Tecnologia Química e Biológica António Xavier (ITQB)RUNSokol, Katarzyna P.Robinson, William E.Oliveira, Ana R.Zacarias, SoniaLee, Chong YongMadden, ChristopherBassegoda, ArnauHirst, JudyPereira, Inês A.C.Reisner, Erwin2020-01-16T23:38:50Z2019-09-042019-09-04T00:00:00Zinfo:eu-repo/semantics/publishedVersioninfo:eu-repo/semantics/article5application/pdfhttp://hdl.handle.net/10362/91347eng0002-7863PURE: 16379771https://doi.org/10.1021/jacs.9b09575info:eu-repo/semantics/openAccessreponame:Repositório Científico de Acesso Aberto de Portugal (Repositórios Cientìficos)instname:Agência para a Sociedade do Conhecimento (UMIC) - FCT - Sociedade da Informaçãoinstacron:RCAAP2024-03-11T04:40:37Zoai:run.unl.pt:10362/91347Portal AgregadorONGhttps://www.rcaap.pt/oai/openaireopendoar:71602024-03-20T03:37:20.076072Repositório Científico de Acesso Aberto de Portugal (Repositórios Cientìficos) - Agência para a Sociedade do Conhecimento (UMIC) - FCT - Sociedade da Informaçãofalse
dc.title.none.fl_str_mv Reversible and Selective Interconversion of Hydrogen and Carbon Dioxide into Formate by a Semiartificial Formate Hydrogenlyase Mimic
title Reversible and Selective Interconversion of Hydrogen and Carbon Dioxide into Formate by a Semiartificial Formate Hydrogenlyase Mimic
spellingShingle Reversible and Selective Interconversion of Hydrogen and Carbon Dioxide into Formate by a Semiartificial Formate Hydrogenlyase Mimic
Sokol, Katarzyna P.
Catalysis
Chemistry(all)
Biochemistry
Colloid and Surface Chemistry
title_short Reversible and Selective Interconversion of Hydrogen and Carbon Dioxide into Formate by a Semiartificial Formate Hydrogenlyase Mimic
title_full Reversible and Selective Interconversion of Hydrogen and Carbon Dioxide into Formate by a Semiartificial Formate Hydrogenlyase Mimic
title_fullStr Reversible and Selective Interconversion of Hydrogen and Carbon Dioxide into Formate by a Semiartificial Formate Hydrogenlyase Mimic
title_full_unstemmed Reversible and Selective Interconversion of Hydrogen and Carbon Dioxide into Formate by a Semiartificial Formate Hydrogenlyase Mimic
title_sort Reversible and Selective Interconversion of Hydrogen and Carbon Dioxide into Formate by a Semiartificial Formate Hydrogenlyase Mimic
author Sokol, Katarzyna P.
author_facet Sokol, Katarzyna P.
Robinson, William E.
Oliveira, Ana R.
Zacarias, Sonia
Lee, Chong Yong
Madden, Christopher
Bassegoda, Arnau
Hirst, Judy
Pereira, Inês A.C.
Reisner, Erwin
author_role author
author2 Robinson, William E.
Oliveira, Ana R.
Zacarias, Sonia
Lee, Chong Yong
Madden, Christopher
Bassegoda, Arnau
Hirst, Judy
Pereira, Inês A.C.
Reisner, Erwin
author2_role author
author
author
author
author
author
author
author
author
dc.contributor.none.fl_str_mv Instituto de Tecnologia Química e Biológica António Xavier (ITQB)
RUN
dc.contributor.author.fl_str_mv Sokol, Katarzyna P.
Robinson, William E.
Oliveira, Ana R.
Zacarias, Sonia
Lee, Chong Yong
Madden, Christopher
Bassegoda, Arnau
Hirst, Judy
Pereira, Inês A.C.
Reisner, Erwin
dc.subject.por.fl_str_mv Catalysis
Chemistry(all)
Biochemistry
Colloid and Surface Chemistry
topic Catalysis
Chemistry(all)
Biochemistry
Colloid and Surface Chemistry
description The biological formate hydrogenlyase (FHL) complex links a formate dehydrogenase (FDH) to a hydrogenase (H2ase) and produces H2 and CO2 from formate via mixed-acid fermentation in Escherichia coli. Here, we describe an electrochemical and a colloidal semiartificial FHL system that consists of an FDH and a H2ase immobilized on conductive indium tin oxide (ITO) as an electron relay. These in vitro systems benefit from the efficient wiring of a highly active enzyme pair and allow for the reversible conversion of formate to H2 and CO2 under ambient temperature and pressure. The hybrid systems provide a template for the design of synthetic catalysts and surpass the FHL complex in vivo by storing and releasing H2 on demand by interconverting CO2/H2 and formate with minimal bias in either direction.
publishDate 2019
dc.date.none.fl_str_mv 2019-09-04
2019-09-04T00:00:00Z
2020-01-16T23:38:50Z
dc.type.status.fl_str_mv info:eu-repo/semantics/publishedVersion
dc.type.driver.fl_str_mv info:eu-repo/semantics/article
format article
status_str publishedVersion
dc.identifier.uri.fl_str_mv http://hdl.handle.net/10362/91347
url http://hdl.handle.net/10362/91347
dc.language.iso.fl_str_mv eng
language eng
dc.relation.none.fl_str_mv 0002-7863
PURE: 16379771
https://doi.org/10.1021/jacs.9b09575
dc.rights.driver.fl_str_mv info:eu-repo/semantics/openAccess
eu_rights_str_mv openAccess
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repository.name.fl_str_mv Repositório Científico de Acesso Aberto de Portugal (Repositórios Cientìficos) - Agência para a Sociedade do Conhecimento (UMIC) - FCT - Sociedade da Informação
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