In-Depth 2D NMR Study of Lignin Modification During Pretreatment of Eucalyptus Wood with Laccase and Mediators

20 páginas.-- 7 figuras.-- 6 tablas.-- 37 referencias.-- Artículo en Prensa

Detalles Bibliográficos
Autores: Rico Campos, Alejandro, Rencoret, Jorge, Río Andrade, José Carlos del, Martínez, Ángel T., Gutiérrez Suárez, Ana
Tipo de recurso: artículo
Estado:Versión enviada para evaluación y publicación
Fecha de publicación:2014
País:España
Institución:Consejo Superior de Investigaciones Científicas (CSIC)
Repositorio:DIGITAL.CSIC. Repositorio Institucional del CSIC
OAI Identifier:oai:digital.csic.es:10261/101255
Acceso en línea:http://hdl.handle.net/10261/101255
Access Level:acceso abierto
Palabra clave:2D NMR
Bioethanol
Enzymatic delignification
Laccase mediator
Lignin
S/G ratio
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spelling In-Depth 2D NMR Study of Lignin Modification During Pretreatment of Eucalyptus Wood with Laccase and MediatorsRico Campos, AlejandroRencoret, JorgeRío Andrade, José Carlos delMartínez, Ángel T.Gutiérrez Suárez, Ana2D NMRBioethanolEnzymatic delignificationLaccase mediatorLigninS/G ratio20 páginas.-- 7 figuras.-- 6 tablas.-- 37 referencias.-- Artículo en PrensaEucalypt feedstock was pretreated with Myceliophthora thermophila laccase and methyl syringate, as mediator, in a multistage sequence consisting of successive enzymatic and alkaline peroxide stages, directly on the ground wood. Lignin modification was studied by two-dimensional (2D) nuclear magnetic resonance (NMR) of wood (at the gel state) after each stage of the sequence. Decrease of guaiacyl and syringyl lignin units (with preferential removal of the former) and aliphatic (mainly β-O-4′-linked) side chains was observed along the sequence, without a substantial change in polysaccharide cross-signals along the sequence, was observed. However, the most noticeable modification was the formation of Cα-oxidized syringyl units in the enzymatic stages, which were partially removed in the alkaline extractions. Further insight was attained by 2D NMR of the cellulolytic-enzyme lignins, isolated from the pretreated samples, and the filtrates from the different stages. Additionally, a comparison of eucalypt delignification with the high redox potential laccase from Pycnoporus cinnabarinus in the presence of the synthetic mediator 1-hydroxybenzotriazole was carried out. Wood delignification already occurred at the first cycle of the pretreatment with P. cinnabarinus laccase and 1-hydroxybenzotriazole, which directly correlated with increases in glucose (~10 %) yields after enzymatic hydrolysis. In contrast, the first cycle of pretreatment with M. thermophila laccase and methyl syringate did not produce any delignification or saccharification improvement. However, at the end of the sequence, similar delignification (~50 %) of eucalypt feedstock and increases (~30 %) in glucose yields were attained in both laccase-mediator pretreatments. Finally, the influence of lignin content and the ratio of its syringyl and guaiacyl units on recalcitrance of eucalypt feedstock to enzymatic saccharification is discussed.This study was funded by the INDOX (KBBE-2013-7-613549) EU-project and the LIGNOCELL (AGL2011-25379) and HIPOP (BIO2011-2669) Spanish MICINN projects (co-financed by FEDER funds). J. Rencoret acknowledges the CSIC JAE-Doc contract of the program “Junta para la Ampliación de Estudios” co-financed by the European Social Fund (ESF). H. Lund and L. Kalum from Novozymes (Bagsvaerd, Denmark) are acknowledged for the cellulases (Celluclast and Novozym 188) and the M. thermophila laccase, Beldem (Andenne, Belgium) for the P. cinnabarinus laccase and J. Romero (ENCE, Spain) for the eucalypt wood samples. Manuel Angulo (CITIUS, University of Seville) is acknowledged for providing technical assistance in the NMR analyses.Peer reviewedSpringer NatureConsejo Superior de Investigaciones Científicas [https://ror.org/02gfc7t72]201420142015info:eu-repo/semantics/articlehttp://purl.org/coar/resource_type/c_6501Preprintinfo:eu-repo/semantics/submittedVersionhttp://hdl.handle.net/10261/101255reponame:DIGITAL.CSIC. Repositorio Institucional del CSICinstname:Consejo Superior de Investigaciones Científicas (CSIC)Ingléshttp://dx.doi.org/10.1007/s12155-014-9505-xSíinfo:eu-repo/semantics/openAccessoai:digital.csic.es:10261/1012552026-05-22T06:33:51Z
dc.title.none.fl_str_mv In-Depth 2D NMR Study of Lignin Modification During Pretreatment of Eucalyptus Wood with Laccase and Mediators
title In-Depth 2D NMR Study of Lignin Modification During Pretreatment of Eucalyptus Wood with Laccase and Mediators
spellingShingle In-Depth 2D NMR Study of Lignin Modification During Pretreatment of Eucalyptus Wood with Laccase and Mediators
Rico Campos, Alejandro
2D NMR
Bioethanol
Enzymatic delignification
Laccase mediator
Lignin
S/G ratio
title_short In-Depth 2D NMR Study of Lignin Modification During Pretreatment of Eucalyptus Wood with Laccase and Mediators
title_full In-Depth 2D NMR Study of Lignin Modification During Pretreatment of Eucalyptus Wood with Laccase and Mediators
title_fullStr In-Depth 2D NMR Study of Lignin Modification During Pretreatment of Eucalyptus Wood with Laccase and Mediators
title_full_unstemmed In-Depth 2D NMR Study of Lignin Modification During Pretreatment of Eucalyptus Wood with Laccase and Mediators
title_sort In-Depth 2D NMR Study of Lignin Modification During Pretreatment of Eucalyptus Wood with Laccase and Mediators
dc.creator.none.fl_str_mv Rico Campos, Alejandro
Rencoret, Jorge
Río Andrade, José Carlos del
Martínez, Ángel T.
Gutiérrez Suárez, Ana
author Rico Campos, Alejandro
author_facet Rico Campos, Alejandro
Rencoret, Jorge
Río Andrade, José Carlos del
Martínez, Ángel T.
Gutiérrez Suárez, Ana
author_role author
author2 Rencoret, Jorge
Río Andrade, José Carlos del
Martínez, Ángel T.
Gutiérrez Suárez, Ana
author2_role author
author
author
author
dc.contributor.none.fl_str_mv Consejo Superior de Investigaciones Científicas [https://ror.org/02gfc7t72]
dc.subject.none.fl_str_mv 2D NMR
Bioethanol
Enzymatic delignification
Laccase mediator
Lignin
S/G ratio
topic 2D NMR
Bioethanol
Enzymatic delignification
Laccase mediator
Lignin
S/G ratio
description 20 páginas.-- 7 figuras.-- 6 tablas.-- 37 referencias.-- Artículo en Prensa
publishDate 2014
dc.date.none.fl_str_mv 2014
2014
2015
dc.type.none.fl_str_mv info:eu-repo/semantics/article
http://purl.org/coar/resource_type/c_6501
Preprint
info:eu-repo/semantics/submittedVersion
format article
status_str submittedVersion
dc.identifier.none.fl_str_mv http://hdl.handle.net/10261/101255
url http://hdl.handle.net/10261/101255
dc.language.none.fl_str_mv Inglés
language_invalid_str_mv Inglés
dc.relation.none.fl_str_mv http://dx.doi.org/10.1007/s12155-014-9505-x
Sí
dc.rights.none.fl_str_mv info:eu-repo/semantics/openAccess
eu_rights_str_mv openAccess
dc.publisher.none.fl_str_mv Springer Nature
publisher.none.fl_str_mv Springer Nature
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 15.812429

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