Cargando…

A structured understanding of cellobiohydrolase I binding to poplar lignin fractions after dilute acid pretreatment

BACKGROUND: Cellulase adsorption to lignin is considered a cost barrier for bioethanol production; however, its detailed association mechanism is still not fully understood. In this study, two natural poplar variants with high and low sugar release performance were selected as the low and high recal...

Descripción completa

Detalles Bibliográficos
Autores principales: Yao, Lan, Yoo, Chang Geun, Meng, Xianzhi, Li, Mi, Pu, Yunqiao, Ragauskas, Arthur J., Yang, Haitao
Formato: Online Artículo Texto
Lenguaje:English
Publicado: BioMed Central 2018
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC5883885/
https://www.ncbi.nlm.nih.gov/pubmed/29632555
http://dx.doi.org/10.1186/s13068-018-1087-y
_version_ 1783311740054798336
author Yao, Lan
Yoo, Chang Geun
Meng, Xianzhi
Li, Mi
Pu, Yunqiao
Ragauskas, Arthur J.
Yang, Haitao
author_facet Yao, Lan
Yoo, Chang Geun
Meng, Xianzhi
Li, Mi
Pu, Yunqiao
Ragauskas, Arthur J.
Yang, Haitao
author_sort Yao, Lan
collection PubMed
description BACKGROUND: Cellulase adsorption to lignin is considered a cost barrier for bioethanol production; however, its detailed association mechanism is still not fully understood. In this study, two natural poplar variants with high and low sugar release performance were selected as the low and high recalcitrant raw materials (named L and H, respectively). Three different lignin fractions were extracted using ethanol, followed by p-dioxane and then cellulase treatment from the dilute acid pretreated poplar solids (fraction 1, 2, and 3, respectively). RESULTS: Each lignin fraction had different physicochemical properties. Ethanol-extracted lignin had the lowest weight average molecular weight, while the molecular weights for the other two lignin fractions were similar. (31)P NMR analysis revealed that lignin fraction with higher molecular weight contained more aliphatic hydroxyl groups and less phenolic hydroxyl groups. Semi-quantitative analysis by 2D HSQC NMR indicated that the lignin fractions isolated from the natural variants had different contents of syringyl (S), guaiacyl (G) and interunit linkages. Lignin extracted by ethanol contained the largest amount of S units, the smallest amounts of G and p-hydroxybenzoate (PB) subunits, while the contents of these lignin subunits in the other two lignin fractions were similar. The lignin fraction obtained after cellulase treatment was primarily comprised of β-O-4 linkages with small amounts of β-5 and β–β linkages. The binding strength of these three lignin fractions obtained by Langmuir equations were in the order of L(1) > L(3) > L(2) for the low recalcitrance poplar and H(1) > H(2) > H(3) for the high recalcitrance poplar. CONCLUSIONS: Overall, adsorption ability of lignin was correlated with the sugar release of poplar. Structural features of lignin were associated with its binding to CBH. For natural poplar variants, lignin fractions with lower molecular weight and polydispersity index (PDI) exhibited more CBH adsorption ability. Lignins with more phenolic hydroxyl groups had higher CBH binding strength. It was also found that lignin fractions with more condensed aromatics adsorbed more CBH likely attributed to stronger hydrophobic interactions. ELECTRONIC SUPPLEMENTARY MATERIAL: The online version of this article (10.1186/s13068-018-1087-y) contains supplementary material, which is available to authorized users.
format Online
Article
Text
id pubmed-5883885
institution National Center for Biotechnology Information
language English
publishDate 2018
publisher BioMed Central
record_format MEDLINE/PubMed
spelling pubmed-58838852018-04-09 A structured understanding of cellobiohydrolase I binding to poplar lignin fractions after dilute acid pretreatment Yao, Lan Yoo, Chang Geun Meng, Xianzhi Li, Mi Pu, Yunqiao Ragauskas, Arthur J. Yang, Haitao Biotechnol Biofuels Research BACKGROUND: Cellulase adsorption to lignin is considered a cost barrier for bioethanol production; however, its detailed association mechanism is still not fully understood. In this study, two natural poplar variants with high and low sugar release performance were selected as the low and high recalcitrant raw materials (named L and H, respectively). Three different lignin fractions were extracted using ethanol, followed by p-dioxane and then cellulase treatment from the dilute acid pretreated poplar solids (fraction 1, 2, and 3, respectively). RESULTS: Each lignin fraction had different physicochemical properties. Ethanol-extracted lignin had the lowest weight average molecular weight, while the molecular weights for the other two lignin fractions were similar. (31)P NMR analysis revealed that lignin fraction with higher molecular weight contained more aliphatic hydroxyl groups and less phenolic hydroxyl groups. Semi-quantitative analysis by 2D HSQC NMR indicated that the lignin fractions isolated from the natural variants had different contents of syringyl (S), guaiacyl (G) and interunit linkages. Lignin extracted by ethanol contained the largest amount of S units, the smallest amounts of G and p-hydroxybenzoate (PB) subunits, while the contents of these lignin subunits in the other two lignin fractions were similar. The lignin fraction obtained after cellulase treatment was primarily comprised of β-O-4 linkages with small amounts of β-5 and β–β linkages. The binding strength of these three lignin fractions obtained by Langmuir equations were in the order of L(1) > L(3) > L(2) for the low recalcitrance poplar and H(1) > H(2) > H(3) for the high recalcitrance poplar. CONCLUSIONS: Overall, adsorption ability of lignin was correlated with the sugar release of poplar. Structural features of lignin were associated with its binding to CBH. For natural poplar variants, lignin fractions with lower molecular weight and polydispersity index (PDI) exhibited more CBH adsorption ability. Lignins with more phenolic hydroxyl groups had higher CBH binding strength. It was also found that lignin fractions with more condensed aromatics adsorbed more CBH likely attributed to stronger hydrophobic interactions. ELECTRONIC SUPPLEMENTARY MATERIAL: The online version of this article (10.1186/s13068-018-1087-y) contains supplementary material, which is available to authorized users. BioMed Central 2018-04-04 /pmc/articles/PMC5883885/ /pubmed/29632555 http://dx.doi.org/10.1186/s13068-018-1087-y Text en © The Author(s) 2018 Open AccessThis article is distributed under the terms of the Creative Commons Attribution 4.0 International License (http://creativecommons.org/licenses/by/4.0/), which permits unrestricted use, distribution, and reproduction in any medium, provided you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The Creative Commons Public Domain Dedication waiver (http://creativecommons.org/publicdomain/zero/1.0/) applies to the data made available in this article, unless otherwise stated.
spellingShingle Research
Yao, Lan
Yoo, Chang Geun
Meng, Xianzhi
Li, Mi
Pu, Yunqiao
Ragauskas, Arthur J.
Yang, Haitao
A structured understanding of cellobiohydrolase I binding to poplar lignin fractions after dilute acid pretreatment
title A structured understanding of cellobiohydrolase I binding to poplar lignin fractions after dilute acid pretreatment
title_full A structured understanding of cellobiohydrolase I binding to poplar lignin fractions after dilute acid pretreatment
title_fullStr A structured understanding of cellobiohydrolase I binding to poplar lignin fractions after dilute acid pretreatment
title_full_unstemmed A structured understanding of cellobiohydrolase I binding to poplar lignin fractions after dilute acid pretreatment
title_short A structured understanding of cellobiohydrolase I binding to poplar lignin fractions after dilute acid pretreatment
title_sort structured understanding of cellobiohydrolase i binding to poplar lignin fractions after dilute acid pretreatment
topic Research
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC5883885/
https://www.ncbi.nlm.nih.gov/pubmed/29632555
http://dx.doi.org/10.1186/s13068-018-1087-y
work_keys_str_mv AT yaolan astructuredunderstandingofcellobiohydrolaseibindingtopoplarligninfractionsafterdiluteacidpretreatment
AT yoochanggeun astructuredunderstandingofcellobiohydrolaseibindingtopoplarligninfractionsafterdiluteacidpretreatment
AT mengxianzhi astructuredunderstandingofcellobiohydrolaseibindingtopoplarligninfractionsafterdiluteacidpretreatment
AT limi astructuredunderstandingofcellobiohydrolaseibindingtopoplarligninfractionsafterdiluteacidpretreatment
AT puyunqiao astructuredunderstandingofcellobiohydrolaseibindingtopoplarligninfractionsafterdiluteacidpretreatment
AT ragauskasarthurj astructuredunderstandingofcellobiohydrolaseibindingtopoplarligninfractionsafterdiluteacidpretreatment
AT yanghaitao astructuredunderstandingofcellobiohydrolaseibindingtopoplarligninfractionsafterdiluteacidpretreatment
AT yaolan structuredunderstandingofcellobiohydrolaseibindingtopoplarligninfractionsafterdiluteacidpretreatment
AT yoochanggeun structuredunderstandingofcellobiohydrolaseibindingtopoplarligninfractionsafterdiluteacidpretreatment
AT mengxianzhi structuredunderstandingofcellobiohydrolaseibindingtopoplarligninfractionsafterdiluteacidpretreatment
AT limi structuredunderstandingofcellobiohydrolaseibindingtopoplarligninfractionsafterdiluteacidpretreatment
AT puyunqiao structuredunderstandingofcellobiohydrolaseibindingtopoplarligninfractionsafterdiluteacidpretreatment
AT ragauskasarthurj structuredunderstandingofcellobiohydrolaseibindingtopoplarligninfractionsafterdiluteacidpretreatment
AT yanghaitao structuredunderstandingofcellobiohydrolaseibindingtopoplarligninfractionsafterdiluteacidpretreatment