Light Boosts the Activity of Novel LPMO from Aspergillus fumigatus Leading to Oxidative Cleavage of Cellulose and Hemicellulose
Autor(a) principal: | |
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Data de Publicação: | 2022 |
Outros Autores: | , , , , , , |
Tipo de documento: | Artigo |
Idioma: | eng |
Título da fonte: | Repositório Institucional da UNESP |
Texto Completo: | http://dx.doi.org/10.1021/acssuschemeng.2c06281 http://hdl.handle.net/11449/246514 |
Resumo: | Lytic polysaccharide monooxygenases (LPMOs) are copper-dependent enzymes that potentiate the deconstruction of polysaccharides through an oxidative mechanism. The oxidative catalysis of LPMOs is dependent on a reductant to promote the divalent copper ion in a metalloenzyme to its monovalent state. The reported molecules that can activate LPMOs are organic compounds of low molecular weight, enzymes, lignin and lignin-derived compounds, and, recently, photosynthetic pigments. This work reports the functional characterization and the computational modeling of the three-dimensional structure of a novel LPMO from Aspergillus fumigatus var. niveus (AfAA9C). AfAA9C shows the ability to oxidize glucose residues in the cellulose chain at C1- and C4-carbon, being the first reported LPMO from A. fumigatus active on xyloglucan and capable of being activated by light. The evaluation of electron donors coupled to chlorophyllin + light photosystems allowed to elucidate the existence of a collaborative effect between a chemical reducing agent and light-induced electron transfer systems promoting changes in LPMO activity, which is reducing agent-type-dependent. The results suggest that the preference of AfAA9C for a specific reducing agent is altered when the compound is associated with the photosystem due to H2O2generation. These findings are of general importance for the utilization of LPMOs in reactions applying photobiocatalysis and in sustainable industrial processes such as biomass depolymerization. copy; 2022 American Chemical Society. |
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Light Boosts the Activity of Novel LPMO from Aspergillus fumigatus Leading to Oxidative Cleavage of Cellulose and Hemicellulosecelluloselytic polysaccharide monooxygenasesphotobiocatalysisxyloglucanLytic polysaccharide monooxygenases (LPMOs) are copper-dependent enzymes that potentiate the deconstruction of polysaccharides through an oxidative mechanism. The oxidative catalysis of LPMOs is dependent on a reductant to promote the divalent copper ion in a metalloenzyme to its monovalent state. The reported molecules that can activate LPMOs are organic compounds of low molecular weight, enzymes, lignin and lignin-derived compounds, and, recently, photosynthetic pigments. This work reports the functional characterization and the computational modeling of the three-dimensional structure of a novel LPMO from Aspergillus fumigatus var. niveus (AfAA9C). AfAA9C shows the ability to oxidize glucose residues in the cellulose chain at C1- and C4-carbon, being the first reported LPMO from A. fumigatus active on xyloglucan and capable of being activated by light. The evaluation of electron donors coupled to chlorophyllin + light photosystems allowed to elucidate the existence of a collaborative effect between a chemical reducing agent and light-induced electron transfer systems promoting changes in LPMO activity, which is reducing agent-type-dependent. The results suggest that the preference of AfAA9C for a specific reducing agent is altered when the compound is associated with the photosystem due to H2O2generation. These findings are of general importance for the utilization of LPMOs in reactions applying photobiocatalysis and in sustainable industrial processes such as biomass depolymerization. copy; 2022 American Chemical Society.Synthetic and Molecular Biology Laboratory Department of Biotechnology Lorena School of Engineering University of São Paulo, SPDepartment of Physics and Applied Sciences São Carlos Institute of Physics University of São Paulo, SPPhotoBiocatalysis Unit-CPBL and BTL École Interfacultaire de Bioingénieurs (EIB) Université Libre de BruxellesDepartment of Physics Institute of Biosciences Humanities and Exact Sciences São Paulo State University (UNESP), SPDepartment of Physics Institute of Biosciences Humanities and Exact Sciences São Paulo State University (UNESP), SPUniversidade de São Paulo (USP)Université Libre de BruxellesUniversidade Estadual Paulista (UNESP)Velasco, JosmanSepulchro, Ana Gabriela V.Higasi, Paula M. R.Pellegrini, Vanessa O. A.Cannella, DavidDe Oliveira, Leandro Cristante [UNESP]Polikarpov, IgorSegato, Fernando2023-07-29T12:43:07Z2023-07-29T12:43:07Z2022-12-19info:eu-repo/semantics/publishedVersioninfo:eu-repo/semantics/article16969-16984http://dx.doi.org/10.1021/acssuschemeng.2c06281ACS Sustainable Chemistry and Engineering, v. 10, n. 50, p. 16969-16984, 2022.2168-0485http://hdl.handle.net/11449/24651410.1021/acssuschemeng.2c062812-s2.0-85144515125Scopusreponame:Repositório Institucional da UNESPinstname:Universidade Estadual Paulista (UNESP)instacron:UNESPengACS Sustainable Chemistry and Engineeringinfo:eu-repo/semantics/openAccess2023-07-29T12:43:07Zoai:repositorio.unesp.br:11449/246514Repositório InstitucionalPUBhttp://repositorio.unesp.br/oai/requestopendoar:29462024-08-05T20:30:28.310715Repositório Institucional da UNESP - Universidade Estadual Paulista (UNESP)false |
dc.title.none.fl_str_mv |
Light Boosts the Activity of Novel LPMO from Aspergillus fumigatus Leading to Oxidative Cleavage of Cellulose and Hemicellulose |
title |
Light Boosts the Activity of Novel LPMO from Aspergillus fumigatus Leading to Oxidative Cleavage of Cellulose and Hemicellulose |
spellingShingle |
Light Boosts the Activity of Novel LPMO from Aspergillus fumigatus Leading to Oxidative Cleavage of Cellulose and Hemicellulose Velasco, Josman cellulose lytic polysaccharide monooxygenases photobiocatalysis xyloglucan |
title_short |
Light Boosts the Activity of Novel LPMO from Aspergillus fumigatus Leading to Oxidative Cleavage of Cellulose and Hemicellulose |
title_full |
Light Boosts the Activity of Novel LPMO from Aspergillus fumigatus Leading to Oxidative Cleavage of Cellulose and Hemicellulose |
title_fullStr |
Light Boosts the Activity of Novel LPMO from Aspergillus fumigatus Leading to Oxidative Cleavage of Cellulose and Hemicellulose |
title_full_unstemmed |
Light Boosts the Activity of Novel LPMO from Aspergillus fumigatus Leading to Oxidative Cleavage of Cellulose and Hemicellulose |
title_sort |
Light Boosts the Activity of Novel LPMO from Aspergillus fumigatus Leading to Oxidative Cleavage of Cellulose and Hemicellulose |
author |
Velasco, Josman |
author_facet |
Velasco, Josman Sepulchro, Ana Gabriela V. Higasi, Paula M. R. Pellegrini, Vanessa O. A. Cannella, David De Oliveira, Leandro Cristante [UNESP] Polikarpov, Igor Segato, Fernando |
author_role |
author |
author2 |
Sepulchro, Ana Gabriela V. Higasi, Paula M. R. Pellegrini, Vanessa O. A. Cannella, David De Oliveira, Leandro Cristante [UNESP] Polikarpov, Igor Segato, Fernando |
author2_role |
author author author author author author author |
dc.contributor.none.fl_str_mv |
Universidade de São Paulo (USP) Université Libre de Bruxelles Universidade Estadual Paulista (UNESP) |
dc.contributor.author.fl_str_mv |
Velasco, Josman Sepulchro, Ana Gabriela V. Higasi, Paula M. R. Pellegrini, Vanessa O. A. Cannella, David De Oliveira, Leandro Cristante [UNESP] Polikarpov, Igor Segato, Fernando |
dc.subject.por.fl_str_mv |
cellulose lytic polysaccharide monooxygenases photobiocatalysis xyloglucan |
topic |
cellulose lytic polysaccharide monooxygenases photobiocatalysis xyloglucan |
description |
Lytic polysaccharide monooxygenases (LPMOs) are copper-dependent enzymes that potentiate the deconstruction of polysaccharides through an oxidative mechanism. The oxidative catalysis of LPMOs is dependent on a reductant to promote the divalent copper ion in a metalloenzyme to its monovalent state. The reported molecules that can activate LPMOs are organic compounds of low molecular weight, enzymes, lignin and lignin-derived compounds, and, recently, photosynthetic pigments. This work reports the functional characterization and the computational modeling of the three-dimensional structure of a novel LPMO from Aspergillus fumigatus var. niveus (AfAA9C). AfAA9C shows the ability to oxidize glucose residues in the cellulose chain at C1- and C4-carbon, being the first reported LPMO from A. fumigatus active on xyloglucan and capable of being activated by light. The evaluation of electron donors coupled to chlorophyllin + light photosystems allowed to elucidate the existence of a collaborative effect between a chemical reducing agent and light-induced electron transfer systems promoting changes in LPMO activity, which is reducing agent-type-dependent. The results suggest that the preference of AfAA9C for a specific reducing agent is altered when the compound is associated with the photosystem due to H2O2generation. These findings are of general importance for the utilization of LPMOs in reactions applying photobiocatalysis and in sustainable industrial processes such as biomass depolymerization. copy; 2022 American Chemical Society. |
publishDate |
2022 |
dc.date.none.fl_str_mv |
2022-12-19 2023-07-29T12:43:07Z 2023-07-29T12:43:07Z |
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://dx.doi.org/10.1021/acssuschemeng.2c06281 ACS Sustainable Chemistry and Engineering, v. 10, n. 50, p. 16969-16984, 2022. 2168-0485 http://hdl.handle.net/11449/246514 10.1021/acssuschemeng.2c06281 2-s2.0-85144515125 |
url |
http://dx.doi.org/10.1021/acssuschemeng.2c06281 http://hdl.handle.net/11449/246514 |
identifier_str_mv |
ACS Sustainable Chemistry and Engineering, v. 10, n. 50, p. 16969-16984, 2022. 2168-0485 10.1021/acssuschemeng.2c06281 2-s2.0-85144515125 |
dc.language.iso.fl_str_mv |
eng |
language |
eng |
dc.relation.none.fl_str_mv |
ACS Sustainable Chemistry and Engineering |
dc.rights.driver.fl_str_mv |
info:eu-repo/semantics/openAccess |
eu_rights_str_mv |
openAccess |
dc.format.none.fl_str_mv |
16969-16984 |
dc.source.none.fl_str_mv |
Scopus reponame:Repositório Institucional da UNESP instname:Universidade Estadual Paulista (UNESP) instacron:UNESP |
instname_str |
Universidade Estadual Paulista (UNESP) |
instacron_str |
UNESP |
institution |
UNESP |
reponame_str |
Repositório Institucional da UNESP |
collection |
Repositório Institucional da UNESP |
repository.name.fl_str_mv |
Repositório Institucional da UNESP - Universidade Estadual Paulista (UNESP) |
repository.mail.fl_str_mv |
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1808129211987132416 |