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

doi:10.1186/s13068-018-1087-y

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

Journal Article · Wed Apr 04 00:00:00 EDT 2018 · Biotechnology for Biofuels

DOI:https://doi.org/10.1186/s13068-018-1087-y· OSTI ID:1618719

Yao, Lan; Yoo, Chang Geun; Meng, Xianzhi; Li, Mi; Pu, Yunqiao;

; Yang, Haitao

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. 31P 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 L1 > L3 > L2 for the low recalcitrance poplar and H1 > H2 > H3 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.

View Journal Article

Cite

Export

Save

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1618719

Alternate ID(s):: OSTI ID: 1436929

Journal Information:: Biotechnology for Biofuels, Journal Name: Biotechnology for Biofuels Vol. 11 Journal Issue: 1; ISSN 1754-6834

Publisher:: Springer Science + Business MediaCopyright Statement

Country of Publication:: Netherlands

Language:: English

Citation Metrics:

Cited by: 23 works

Citation information provided by
Web of Science

References (41)

Lignin Valorization: Improving Lignin Processing in the Biorefinery Ragauskas, A. J.; Beckham, G. T.; Biddy, M. J. Science, Vol. 344, Issue 6185, p. 1246843-1246843 https://doi.org/10.1126/science.1246843	journal	May 2014
Chemical transformations of Populus trichocarpa during dilute acid pretreatment Cao, Shilin; Pu, Yunqiao; Studer, Michael RSC Advances, Vol. 2, Issue 29 https://doi.org/10.1039/c2ra22045h	journal	January 2012
New Insights into the Structural Organization of the Plant Polymer Lignin RadotiĆ, Ksenija; MiĆIĆ, Miodrag; JeremiĆ, Milorad Annals of the New York Academy of Sciences, Vol. 1048, Issue 1 https://doi.org/10.1196/annals.1342.020	journal	June 2005
Insights of biomass recalcitrance in natural Populus trichocarpa variants for biomass conversion Yoo, Chang Geun; Yang, Yongil; Pu, Yunqiao Green Chemistry, Vol. 19, Issue 22 https://doi.org/10.1039/C7GC02219K	journal	January 2017
Application of quantitative 31P NMR in biomass lignin and biofuel precursors characterization Pu, Yunqiao; Cao, Shilin; Ragauskas, Arthur J. Energy & Environmental Science, Vol. 4, Issue 9 https://doi.org/10.1039/c1ee01201k	journal	January 2011
Fractionation of Organosolv Lignin Using Acetone:Water and Properties of the Obtained Fractions Sadeghifar, Hasan; Wells, Tyrone; Le, Rosemary Khuu ACS Sustainable Chemistry & Engineering, Vol. 5, Issue 1 https://doi.org/10.1021/acssuschemeng.6b01955	journal	November 2016
Mutational Effects on the Catalytic Mechanism of Cellobiohydrolase I from Trichoderma reesei Yan, Shihai; Li, Tong; Yao, Lishan The Journal of Physical Chemistry B, Vol. 115, Issue 17 https://doi.org/10.1021/jp200384m	journal	May 2011
Lignin-enzyme interaction: Mechanism, mitigation approach, modeling, and research prospects Li, Xiang; Zheng, Yi Biotechnology Advances, Vol. 35, Issue 4 https://doi.org/10.1016/j.biotechadv.2017.03.010	journal	July 2017
Effect of Lignin Chemistry on the Enzymatic Hydrolysis of Woody Biomass Yu, Zhiying; Gwak, Ki-Seob; Treasure, Trevor ChemSusChem, Vol. 7, Issue 7 https://doi.org/10.1002/cssc.201400042	journal	June 2014
Structural transformation of hemicelluloses and lignin from triploid poplar during acid-pretreatment based biorefinery process Wang, Kun; Yang, Haiyan; Yao, Xi Bioresource Technology, Vol. 116 https://doi.org/10.1016/j.biortech.2012.04.028	journal	July 2012
Lignin isolated from steam-exploded eucalyptus wood chips by phase separation and its affinity to Trichoderma reesei cellulase Nonaka, Hiroshi; Kobayashi, Ai; Funaoka, Masamitsu Bioresource Technology, Vol. 140 https://doi.org/10.1016/j.biortech.2013.04.109	journal	July 2013
Investigation of lignin deposition on cellulose during hydrothermal pretreatment, its effect on cellulose hydrolysis, and underlying mechanisms: Investigation of Lignin Deposition on Cellulose Li, Hongjia; Pu, Yunqiao; Kumar, Rajeev Biotechnology and Bioengineering, Vol. 111, Issue 3 https://doi.org/10.1002/bit.25108	journal	October 2013
Adsorption and mechanism of cellulase enzymes onto lignin isolated from corn stover pretreated with liquid hot water Lu, Xianqin; Zheng, Xiaoju; Li, Xuezhi Biotechnology for Biofuels, Vol. 9, Issue 1 https://doi.org/10.1186/s13068-016-0531-0	journal	June 2016
Adsorption of Trichoderma reesei Cellulase on Softwood Lignin-based Lignophenol Nonaka, Hirosh; Tanaka, Hiroaki; Funaoka, Masamitsu Journal of the Japan Institute of Energy, Vol. 90, Issue 10 https://doi.org/10.3775/jie.90.977	journal	January 2011
Structural Characterization and Comparison of Switchgrass Ball-milled Lignin Before and After Dilute Acid Pretreatment Samuel, Reichel; Pu, Yunqiao; Raman, Babu Applied Biochemistry and Biotechnology, Vol. 162, Issue 1 https://doi.org/10.1007/s12010-009-8749-y	journal	August 2009
Correlation between lignin physicochemical properties and inhibition to enzymatic hydrolysis of cellulose: Lignin Properties and Enzymatic Hydrolysis Yang, Qiang; Pan, Xuejun Biotechnology and Bioengineering, Vol. 113, Issue 6 https://doi.org/10.1002/bit.25903	journal	December 2015
Interactive forces between lignin and cellulase as determined by atomic force microscopy Qin, Chengrong; Clarke, Kimberley; Li, Kecheng Biotechnology for Biofuels, Vol. 7, Issue 1 https://doi.org/10.1186/1754-6834-7-65	journal	January 2014
Comparative study of lignin characteristics from wheat straw obtained by soda-AQ and kraft pretreatment and effect on the following enzymatic hydrolysis process Yang, Haitao; Xie, Yimin; Zheng, Xing Bioresource Technology, Vol. 207 https://doi.org/10.1016/j.biortech.2016.01.123	journal	May 2016
The strong association of condensed phenolic moieties in isolated lignins with their inhibition of enzymatic hydrolysis Sun, Shaolong; Huang, Yang; Sun, Runcang Green Chemistry, Vol. 18, Issue 15 https://doi.org/10.1039/C6GC00685J	journal	January 2016
Inhibition of cellulase, xylanase and β-glucosidase activities by softwood lignin preparations Berlin, Alex; Balakshin, Mikhail; Gilkes, Neil Journal of Biotechnology, Vol. 125, Issue 2, p. 198-209 https://doi.org/10.1016/j.jbiotec.2006.02.021	journal	September 2006
Peroxidase-dependent cross-linking reactions of p-hydroxycinnamates in plant cell walls Ralph, John; Bunzel, Mirko; Marita, Jane M. Phytochemistry Reviews, Vol. 3, Issue 1-2, p. 79-96 https://doi.org/10.1023/B:PHYT.0000047811.13837.fb	journal	January 2004
Differences in the adsorption of enzymes onto lignins from diverse types of lignocellulosic biomass and the underlying mechanism Guo, Fenfen; Shi, Wenjing; Sun, Wan Biotechnology for Biofuels, Vol. 7, Issue 1 https://doi.org/10.1186/1754-6834-7-38	journal	January 2014
Cover Picture: Eco-friendly Energy Storage System: Seawater and Ionic Liquid Electrolyte (ChemSusChem 1/2016) Kim, Jae-Kwang; Mueller, Franziska; Kim, Hyojin ChemSusChem, Vol. 9, Issue 1 https://doi.org/10.1002/cssc.201501673	journal	January 2016
Effects of organosolv and ammonia pretreatments on lignin properties and its inhibition for enzymatic hydrolysis Yoo, Chang Geun; Li, Mi; Meng, Xianzhi Green Chemistry, Vol. 19, Issue 8 https://doi.org/10.1039/C6GC03627A	journal	January 2017
Bisulfite pretreatment changes the structure and properties of oil palm empty fruit bunch to improve enzymatic hydrolysis and bioethanol production Tan, Liping; Sun, Wan; Li, Xuezhi Biotechnology Journal, Vol. 10, Issue 6 https://doi.org/10.1002/biot.201400733	journal	April 2015
Fractionation and physico-chemical analysis of degraded lignins from the black liquor of Eucalyptus pellita KP-AQ pulping Yuan, Tong-Qi; He, Jing; Xu, Feng Polymer Degradation and Stability, Vol. 94, Issue 7 https://doi.org/10.1016/j.polymdegradstab.2009.03.019	journal	July 2009
Adsorption of Trichoderma reesei CBH I and EG II and their catalytic domains on steam pretreated softwood and isolated lignin Palonen, Hetti; Tjerneld, Folke; Zacchi, Guido Journal of Biotechnology, Vol. 107, Issue 1 https://doi.org/10.1016/j.jbiotec.2003.09.011	journal	January 2004
Profiling of Oligolignols Reveals Monolignol Coupling Conditions in Lignifying Poplar Xylem Morreel, Kris; Ralph, John; Kim, Hoon Plant Physiology, Vol. 136, Issue 3 https://doi.org/10.1104/pp.104.049304	journal	October 2004
Mechanism of surfactant effect in enzymatic hydrolysis of lignocellulose Eriksson, Torny; Börjesson, Johan; Tjerneld, Folke Enzyme and Microbial Technology, Vol. 31, Issue 3 https://doi.org/10.1016/S0141-0229(02)00134-5	journal	August 2002
Comparison of hydrothermal, hydrotropic and organosolv pretreatment for improving the enzymatic digestibility of bamboo Mou, Hongyan; Wu, Shubin Cellulose, Vol. 24, Issue 1 https://doi.org/10.1007/s10570-016-1117-5	journal	November 2016
Inhibitory effect of vanillin on cellulase activity in hydrolysis of cellulosic biomass Li, Yun; Qi, Benkun; Wan, Yinhua Bioresource Technology, Vol. 167 https://doi.org/10.1016/j.biortech.2014.06.035	journal	September 2014
Comparison of laboratory delignification methods, their selectivity, and impacts on physiochemical characteristics of cellulosic biomass Kumar, Rajeev; Hu, Fan; Hubbell, Christopher A. Bioresource Technology, Vol. 130 https://doi.org/10.1016/j.biortech.2012.12.028	journal	February 2013
Adsorption of high-purity endo-1,4-β-glucanases from Trichoderma reesei on components of lignocellulosic materials: Cellulose, lignin, and xylan Chernoglazov, Vladimir M.; Ermolova, Olga V.; Klyosov, Anatole A. Enzyme and Microbial Technology, Vol. 10, Issue 8, p. 503-507 https://doi.org/10.1016/0141-0229(88)90029-4	journal	August 1988
Role of Functional Groups in Lignin Inhibition of Enzymatic Hydrolysis of Cellulose to Glucose Pan, Xuejun Journal of Biobased Materials and Bioenergy, Vol. 2, Issue 1 https://doi.org/10.1166/jbmb.2008.005	journal	March 2008
The isolation, characterization and effect of lignin isolated from steam pretreated Douglas-fir on the enzymatic hydrolysis of cellulose Nakagame, Seiji; Chandra, Richard P.; Kadla, John F. Bioresource Technology, Vol. 102, Issue 6 https://doi.org/10.1016/j.biortech.2010.12.082	journal	March 2011
Adsorption of cellobiohydrolases I onto lignin fractions from dilute acid pretreated Broussonetia papyrifera Yao, Lan; Yang, Haitao; Yoo, Chang Geun Bioresource Technology, Vol. 244 https://doi.org/10.1016/j.biortech.2017.08.024	journal	November 2017
Adsorption of enzyme onto lignins of liquid hot water pretreated hardwoods: Enzyme Adsorption by Lignin in Hardwood Ko, Ja Kyong; Ximenes, Eduardo; Kim, Youngmi Biotechnology and Bioengineering, Vol. 112, Issue 3 https://doi.org/10.1002/bit.25359	journal	September 2014
Cellulase adsorption on lignin: A roadblock for economic hydrolysis of biomass Saini, Jitendra Kumar; Patel, Anil Kumar; Adsul, Mukund Renewable Energy, Vol. 98 https://doi.org/10.1016/j.renene.2016.03.089	journal	December 2016
Fractional Precipitation of Softwood Kraft Lignin: Isolation of Narrow Fractions Common to a Variety of Lignins Cui, Chengzhong; Sun, Runkun; Argyropoulos, Dimitris S. ACS Sustainable Chemistry & Engineering, Vol. 2, Issue 4 https://doi.org/10.1021/sc400545d	journal	February 2014
Enhancing the enzymatic hydrolysis of lignocellulosic biomass by increasing the carboxylic acid content of the associated lignin Nakagame, Seiji; Chandra, Richard P.; Kadla, John F. Biotechnology and Bioengineering, Vol. 108, Issue 3 https://doi.org/10.1002/bit.22981	journal	November 2010
Classification of Lignins from Different Botanical Origins by FT-IR Spectroscopy Faix, O. Holzforschung, Vol. 45, Issue s1 https://doi.org/10.1515/hfsg.1991.45.s1.21	journal	January 1991

Cited By (3)

New strategy to elucidate the positive effects of extractable lignin on enzymatic hydrolysis by quartz crystal microbalance with dissipation Lai, Chenhuan; Yang, Bo; Lin, Zihe Biotechnology for Biofuels, Vol. 12, Issue 1 https://doi.org/10.1186/s13068-019-1402-2	journal	March 2019
Lignocellulosic Biomass: Understanding Recalcitrance and Predicting Hydrolysis Zoghlami, Aya; Paës, Gabriel Frontiers in Chemistry, Vol. 7 https://doi.org/10.3389/fchem.2019.00874	journal	December 2019
Unraveling the Fate of Lignin from Eucalyptus and Poplar during Integrated Delignification and Bleaching Wang, Hanmin; Wang, Bing; Sun, Dan ChemSusChem, Vol. 12, Issue 5 https://doi.org/10.1002/cssc.201802592	journal	February 2019

Linked Research (3)

Similar Records

Effects of organosolv and ammonia pretreatments on lignin properties and its inhibition for enzymatic hydrolysis

Journal Article · Wed Apr 05 00:00:00 EDT 2017 · Green Chemistry · OSTI ID:1618719

Yoo, Chang Geun; Li, Mi; Meng, Xianzhi; +2 more

Chemical Transformations of Poplar Lignin during Cosolvent Enhanced Lignocellulosic Fractionation Process

Journal Article · Thu May 24 00:00:00 EDT 2018 · ACS Sustainable Chemistry & Engineering · OSTI ID:1618719

Meng, Xianzhi; Parikh, Aakash; Seemala, Bhogeswararao; +6 more

The Nature of Hololignin

Journal Article · Tue Nov 07 00:00:00 EST 2017 · ACS Sustainable Chemistry & Engineering · OSTI ID:1618719

Meng, Xianzhi; Pu, Yunqiao; Sannigrahi, Poulomi; +3 more

Related Subjects

09 BIOMASS FUELS

MOESM1 of A structured understanding of cellobiohydrolase I binding to poplar lignin fractions after dilute acid pretreatment Yao, Lan; Yoo, Chang; Meng, Xianzhi https://doi.org/10.6084/m9.figshare.6094247 The current record is supplemented by this figure	figure	April 2018
A structured understanding of cellobiohydrolase I binding to poplar lignin fractions after dilute acid pretreatment Yao, Lan; Yoo, Chang; Meng, Xianzhi https://doi.org/10.6084/m9.figshare.c.4059746.v1 The current record is supplemented by this dataset	dataset	April 2018
MOESM1 of A structured understanding of cellobiohydrolase I binding to poplar lignin fractions after dilute acid pretreatment Yao, Lan; Yoo, Chang; Meng, Xianzhi https://doi.org/10.6084/m9.figshare.6094247.v1 The current record is supplemented by this dataset	dataset	April 2018