A new CuZ active form in the catalytic reduction of N2O by nitrous oxide reductase from Pseudomonas nautica

Detalhes bibliográficos
Autor(a) principal: Dell’Acqua, Simone
Data de Publicação: 2010
Outros Autores: Pauleta, Sofia R., Sousa, Patrícia M. Paes de, Monzani, Enrico, Casella, Luigi, Moura, José J. G., Moura, Isabel
Tipo de documento: Artigo
Idioma: eng
Título da fonte: Repositório Científico de Acesso Aberto de Portugal (Repositórios Cientìficos)
Texto Completo: http://hdl.handle.net/10362/8624
Resumo: J Biol Inorg Chem (2010) 15:967–976 DOI 10.1007/s00775-010-0658-6
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spelling A new CuZ active form in the catalytic reduction of N2O by nitrous oxide reductase from Pseudomonas nauticaNitrous oxide reductaseCatalytic mechanismDenitrificationBioelectrochemistryJ Biol Inorg Chem (2010) 15:967–976 DOI 10.1007/s00775-010-0658-6The final step of bacterial denitrification, the two-electron reduction of N2O to N2, is catalyzed by a multi-copper enzyme named nitrous oxide reductase. The catalytic centre of this enzyme is a tetranuclear copper site called CuZ, unique in biological systems. The in vitro reconstruction of the activity requires a slow activation in the presence of the artificial electron donor, reduced methyl viologen, necessary to reduce CuZ from the resting non-active state (1CuII/3CuI) to the fully reduced state (4CuI), in contrast to the turnover cycle, which is very fast. In the present work, the direct reaction of the activated form of Pseudomonas nautica nitrous oxide reductase with stoichiometric amounts of N2O allowed the identification of a new reactive intermediate of the catalytic centre, CuZ°, in the turnover cycle, characterized by an intense absorption band at 680 nm. Moreover, the first mediated electrochemical study of Ps. nautica nitrous oxide reductase with its physiological electron donor, cytochrome c-552, was performed. The intermolecular electron transfer was analysed by cyclic voltammetry, under catalytic conditions, and a second-order rate constant of (5.5 ± 0.9) × 105 M−1 s−1 was determined. Both the reaction of stoichiometric amounts of substrate and the electrochemical studies show that the active CuZ° species, generated in the absence of reductants, can rearrange to the resting non-active CuZ state. In this light, new aspects of the catalytic and activation/inactivation mechanism of the enzyme are discussed.SpringerRUNDell’Acqua, SimonePauleta, Sofia R.Sousa, Patrícia M. Paes deMonzani, EnricoCasella, LuigiMoura, José J. G.Moura, Isabel2013-01-30T12:28:24Z20102010-01-01T00:00:00Zinfo:eu-repo/semantics/publishedVersioninfo:eu-repo/semantics/articleapplication/pdfhttp://hdl.handle.net/10362/8624eng1432-1327info: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:RCAAP2024-03-11T03:41:26Zoai:run.unl.pt:10362/8624Portal AgregadorONGhttps://www.rcaap.pt/oai/openaireopendoar:71602024-03-20T03:18:19.712639Repositório 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 A new CuZ active form in the catalytic reduction of N2O by nitrous oxide reductase from Pseudomonas nautica
title A new CuZ active form in the catalytic reduction of N2O by nitrous oxide reductase from Pseudomonas nautica
spellingShingle A new CuZ active form in the catalytic reduction of N2O by nitrous oxide reductase from Pseudomonas nautica
Dell’Acqua, Simone
Nitrous oxide reductase
Catalytic mechanism
Denitrification
Bioelectrochemistry
title_short A new CuZ active form in the catalytic reduction of N2O by nitrous oxide reductase from Pseudomonas nautica
title_full A new CuZ active form in the catalytic reduction of N2O by nitrous oxide reductase from Pseudomonas nautica
title_fullStr A new CuZ active form in the catalytic reduction of N2O by nitrous oxide reductase from Pseudomonas nautica
title_full_unstemmed A new CuZ active form in the catalytic reduction of N2O by nitrous oxide reductase from Pseudomonas nautica
title_sort A new CuZ active form in the catalytic reduction of N2O by nitrous oxide reductase from Pseudomonas nautica
author Dell’Acqua, Simone
author_facet Dell’Acqua, Simone
Pauleta, Sofia R.
Sousa, Patrícia M. Paes de
Monzani, Enrico
Casella, Luigi
Moura, José J. G.
Moura, Isabel
author_role author
author2 Pauleta, Sofia R.
Sousa, Patrícia M. Paes de
Monzani, Enrico
Casella, Luigi
Moura, José J. G.
Moura, Isabel
author2_role author
author
author
author
author
author
dc.contributor.none.fl_str_mv RUN
dc.contributor.author.fl_str_mv Dell’Acqua, Simone
Pauleta, Sofia R.
Sousa, Patrícia M. Paes de
Monzani, Enrico
Casella, Luigi
Moura, José J. G.
Moura, Isabel
dc.subject.por.fl_str_mv Nitrous oxide reductase
Catalytic mechanism
Denitrification
Bioelectrochemistry
topic Nitrous oxide reductase
Catalytic mechanism
Denitrification
Bioelectrochemistry
description J Biol Inorg Chem (2010) 15:967–976 DOI 10.1007/s00775-010-0658-6
publishDate 2010
dc.date.none.fl_str_mv 2010
2010-01-01T00:00:00Z
2013-01-30T12:28:24Z
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/10362/8624
url http://hdl.handle.net/10362/8624
dc.language.iso.fl_str_mv eng
language eng
dc.relation.none.fl_str_mv 1432-1327
dc.rights.driver.fl_str_mv info:eu-repo/semantics/openAccess
eu_rights_str_mv openAccess
dc.format.none.fl_str_mv application/pdf
dc.publisher.none.fl_str_mv Springer
publisher.none.fl_str_mv Springer
dc.source.none.fl_str_mv reponame:Repositório Científico de Acesso Aberto de Portugal (Repositórios Cientìficos)
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instacron:RCAAP
instname_str Agência para a Sociedade do Conhecimento (UMIC) - FCT - Sociedade da Informação
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