NMR Study on Laccase Polymerization of Kraft Lignin Using Different Enzymes Source

The usage of laccases is a sustainable and environmentally friendly approach to modifying the Kraft lignin structure for use in certain applications. However, the inherent structure of Kraft lignin, as well as that resulting from laccase modification, still presents challenges for fundamental compre...

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Autores: García Fuentevilla, Luisa, Domínguez, Gabriela, Martín Sampedro, Raquel, Hernández, Manuel, Arias, María E., Santos González, José Ignacio, Eugenio, María E.
Tipo de documento: artigo
Data de publicação:2023
País:España
Recursos:Universidad del País Vasco
Repositório:Addi. Archivo Digital para la Docencia y la Investigación
OAI Identifier:oai:addi.ehu.eus:10810/59800
Acesso em linha:http://hdl.handle.net/10810/59800
Access Level:Acceso aberto
Palavra-chave:eucalypt
Kraft lignin
laccase
NMR characterization
polymerization
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spelling NMR Study on Laccase Polymerization of Kraft Lignin Using Different Enzymes SourceGarcía Fuentevilla, LuisaDomínguez, GabrielaMartín Sampedro, RaquelHernández, ManuelArias, María E.Santos González, José IgnacioEugenio, María E.eucalyptKraft ligninlaccaseNMR characterizationpolymerizationThe usage of laccases is a sustainable and environmentally friendly approach to modifying the Kraft lignin structure for use in certain applications. However, the inherent structure of Kraft lignin, as well as that resulting from laccase modification, still presents challenges for fundamental comprehension and successful lignin valorization. In this study, bacterial and fungal laccases were employed to modify eucalypt Kraft lignin. To evaluate the type and range of the chemical and structural changes of laccase-treated lignins, different NMR techniques, including solution 1H and 2D NMR (heteronuclear single quantum correlation (HSQC)), and solid-state 13C NMR, were applied. Size exclusion chromatography and infrared spectroscopy were also used. Interestingly, HSQC analysis showed substantial changes in the oxygenated aliphatic region of lignins, showing an almost complete absence of signals corresponding to side-chains due to laccase depolymerization. Simultaneously, a significant loss of aromatic signals was observed by HSQC and 1H NMR, which was attributed to a deprotonation of the lignin benzenic rings due to polymerization/condensation by laccase reactions. Then, condensed structures, such as α-5′, 5-5′, and 4-O-5′, were detected by HSQC and 13C NMR, supporting the increment in molecular weight, as well as the phenolic content reduction determined in lignins.This research was funded by Comunidad de Madrid via Project SUSTEC-CM S2018/EMT-4348; MCINN/AEI/10.13039/501100011033 and by “ERDF A way of making Europe” via Project RTI2018-096080-B-C22; and MCINN via Project TED2021-132122B-C21.MDPI2023202320232023info:eu-repo/semantics/articleapplication/pdfhttp://hdl.handle.net/10810/59800reponame:Addi. Archivo Digital para la Docencia y la Investigacióninstname:Universidad del País VascoInglésinfo:eu-repo/grantAgreement/MICIU/RTI2018-096080-B-C22/info:eu-repo/grantAgreement/MICINN/TED2021-132122B-C21/https://www.mdpi.com/1422-0067/24/3/2359info:eu-repo/semantics/openAccesshttp://creativecommons.org/licenses/by/4.0/© 2023 by the authors. Licensee MDPI, Basel, Switzerland. This article is an open access article distributed under the terms and conditions of the Creative Commons Attribution (CC BY) license (https://creativecommons.org/licenses/by/ 4.0/).oai:addi.ehu.eus:10810/598002026-06-18T09:23:17Z
dc.title.none.fl_str_mv NMR Study on Laccase Polymerization of Kraft Lignin Using Different Enzymes Source
title NMR Study on Laccase Polymerization of Kraft Lignin Using Different Enzymes Source
spellingShingle NMR Study on Laccase Polymerization of Kraft Lignin Using Different Enzymes Source
García Fuentevilla, Luisa
eucalypt
Kraft lignin
laccase
NMR characterization
polymerization
title_short NMR Study on Laccase Polymerization of Kraft Lignin Using Different Enzymes Source
title_full NMR Study on Laccase Polymerization of Kraft Lignin Using Different Enzymes Source
title_fullStr NMR Study on Laccase Polymerization of Kraft Lignin Using Different Enzymes Source
title_full_unstemmed NMR Study on Laccase Polymerization of Kraft Lignin Using Different Enzymes Source
title_sort NMR Study on Laccase Polymerization of Kraft Lignin Using Different Enzymes Source
dc.creator.none.fl_str_mv García Fuentevilla, Luisa
Domínguez, Gabriela
Martín Sampedro, Raquel
Hernández, Manuel
Arias, María E.
Santos González, José Ignacio
Eugenio, María E.
author García Fuentevilla, Luisa
author_facet García Fuentevilla, Luisa
Domínguez, Gabriela
Martín Sampedro, Raquel
Hernández, Manuel
Arias, María E.
Santos González, José Ignacio
Eugenio, María E.
author_role author
author2 Domínguez, Gabriela
Martín Sampedro, Raquel
Hernández, Manuel
Arias, María E.
Santos González, José Ignacio
Eugenio, María E.
author2_role author
author
author
author
author
author
dc.subject.none.fl_str_mv eucalypt
Kraft lignin
laccase
NMR characterization
polymerization
topic eucalypt
Kraft lignin
laccase
NMR characterization
polymerization
description The usage of laccases is a sustainable and environmentally friendly approach to modifying the Kraft lignin structure for use in certain applications. However, the inherent structure of Kraft lignin, as well as that resulting from laccase modification, still presents challenges for fundamental comprehension and successful lignin valorization. In this study, bacterial and fungal laccases were employed to modify eucalypt Kraft lignin. To evaluate the type and range of the chemical and structural changes of laccase-treated lignins, different NMR techniques, including solution 1H and 2D NMR (heteronuclear single quantum correlation (HSQC)), and solid-state 13C NMR, were applied. Size exclusion chromatography and infrared spectroscopy were also used. Interestingly, HSQC analysis showed substantial changes in the oxygenated aliphatic region of lignins, showing an almost complete absence of signals corresponding to side-chains due to laccase depolymerization. Simultaneously, a significant loss of aromatic signals was observed by HSQC and 1H NMR, which was attributed to a deprotonation of the lignin benzenic rings due to polymerization/condensation by laccase reactions. Then, condensed structures, such as α-5′, 5-5′, and 4-O-5′, were detected by HSQC and 13C NMR, supporting the increment in molecular weight, as well as the phenolic content reduction determined in lignins.
publishDate 2023
dc.date.none.fl_str_mv 2023
2023
2023
2023
dc.type.none.fl_str_mv info:eu-repo/semantics/article
format article
dc.identifier.none.fl_str_mv http://hdl.handle.net/10810/59800
url http://hdl.handle.net/10810/59800
dc.language.none.fl_str_mv Inglés
language_invalid_str_mv Inglés
dc.relation.none.fl_str_mv info:eu-repo/grantAgreement/MICIU/RTI2018-096080-B-C22/
info:eu-repo/grantAgreement/MICINN/TED2021-132122B-C21/
https://www.mdpi.com/1422-0067/24/3/2359
dc.rights.none.fl_str_mv info:eu-repo/semantics/openAccess
http://creativecommons.org/licenses/by/4.0/
eu_rights_str_mv openAccess
rights_invalid_str_mv http://creativecommons.org/licenses/by/4.0/
dc.format.none.fl_str_mv application/pdf
dc.publisher.none.fl_str_mv MDPI
publisher.none.fl_str_mv MDPI
dc.source.none.fl_str_mv reponame:Addi. Archivo Digital para la Docencia y la Investigación
instname:Universidad del País Vasco
instname_str Universidad del País Vasco
reponame_str Addi. Archivo Digital para la Docencia y la Investigación
collection Addi. Archivo Digital para la Docencia y la Investigación
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repository.mail.fl_str_mv
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