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Title: An In-Depth Understanding of Biomass Recalcitrance Using Natural Poplar Variants as the Feedstock

Abstract

In an effort to better understand the biomass recalcitrance, six natural poplar variants were selected as feedstocks based on previous sugar release analysis. We investigated compositional analysis and physicochemical characterizations of these poplars were performed and the correlations between these physicochemical properties and enzymatic hydrolysis yield. Gel permeation chromatography (GPC) and 13C solid state NMR were used to determine the degree of polymerization (DP) and crystallinity index (CrI) of cellulose, and the results along with the sugar release study indicated that cellulose DP likely played a more important role in enzymatic hydrolysis. Simons' stain revealed that the accessible surface area of substrate significantly varied among these variants from 17.3 to 33.2 mg g$$-1\atop{biomass}$$ as reflected by dye adsorption, and cellulose accessibility was shown as one of the major factors governing substrates digestibility. Furthermore, HSQC and 31P NMR analysis detailed the structural features of poplar lignin variants. Overall, cellulose relevant factors appeared to have a stronger correlation with glucose release, if any, than lignin structural features. Lignin structural features, such as a phenolic hydroxyl group and the ratio of syringyl and guaiacyl (S/G), were found to have a more convincing impact on xylose release. Low lignin content, low cellulose DP, and high cellulose accessibility generally favor enzymatic hydrolysis; however, recalcitrance cannot be simply judged on any single substrate factor.

Authors:
 [1];  [2];  [2];  [2];  [3];  [3];  [4];  [4];  [2];  [2];  [2];  [5]
  1. Univ. of Tennessee, Knoxville, TN (United States). Dept. of Chemical and Biomolecular Engineering
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). BioEnergy Science Center and Biosciences Division
  3. Georgia Inst. of Technology, Atlanta, GA (United States). Renewable Bioproducts Inst.
  4. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). BioEnergy Science Center and Biosciences Division; National Renewable Energy Lab. (NREL), Golden, CO (United States)
  5. Univ. of Tennessee, Knoxville, TN (United States). Dept. of Chemical and Biomolecular Engineering and Biosciences Division and Inst. of Agriculture
Publication Date:
Research Org.:
National Renewable Energy Lab. (NREL), Golden, CO (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). BioEnergy Science Center (BESC)
Sponsoring Org.:
USDOE Office of Science (SC), Biological and Environmental Research (BER) (SC-23)
OSTI Identifier:
1343083
Alternate Identifier(s):
OSTI ID: 1337507
Report Number(s):
NREL/JA-5100-67897
Journal ID: ISSN 1864-5631
Grant/Contract Number:  
AC36-08GO28308; AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
ChemSusChem
Additional Journal Information:
Journal Volume: 10; Journal Issue: 1; Journal ID: ISSN 1864-5631
Publisher:
ChemPubSoc Europe
Country of Publication:
United States
Language:
English
Subject:
09 BIOMASS FUELS; biomass recalcitrance; cellulose; crystallinity; degree of polymerization; lignin

Citation Formats

Meng, Xianzhi, Pu, Yunqiao, Yoo, Chang Geun, Li, Mi, Bali, Garima, Park, Doh-Yeon, Gjersing, Erica, Davis, Mark F., Muchero, Wellington, Tuskan, Gerald A., Tschaplinski, Timothy J., and Ragauskas, Arthur J. An In-Depth Understanding of Biomass Recalcitrance Using Natural Poplar Variants as the Feedstock. United States: N. p., 2016. Web. doi:10.1002/cssc.201601303.
Meng, Xianzhi, Pu, Yunqiao, Yoo, Chang Geun, Li, Mi, Bali, Garima, Park, Doh-Yeon, Gjersing, Erica, Davis, Mark F., Muchero, Wellington, Tuskan, Gerald A., Tschaplinski, Timothy J., & Ragauskas, Arthur J. An In-Depth Understanding of Biomass Recalcitrance Using Natural Poplar Variants as the Feedstock. United States. doi:10.1002/cssc.201601303.
Meng, Xianzhi, Pu, Yunqiao, Yoo, Chang Geun, Li, Mi, Bali, Garima, Park, Doh-Yeon, Gjersing, Erica, Davis, Mark F., Muchero, Wellington, Tuskan, Gerald A., Tschaplinski, Timothy J., and Ragauskas, Arthur J. Wed . "An In-Depth Understanding of Biomass Recalcitrance Using Natural Poplar Variants as the Feedstock". United States. doi:10.1002/cssc.201601303. https://www.osti.gov/servlets/purl/1343083.
@article{osti_1343083,
title = {An In-Depth Understanding of Biomass Recalcitrance Using Natural Poplar Variants as the Feedstock},
author = {Meng, Xianzhi and Pu, Yunqiao and Yoo, Chang Geun and Li, Mi and Bali, Garima and Park, Doh-Yeon and Gjersing, Erica and Davis, Mark F. and Muchero, Wellington and Tuskan, Gerald A. and Tschaplinski, Timothy J. and Ragauskas, Arthur J.},
abstractNote = {In an effort to better understand the biomass recalcitrance, six natural poplar variants were selected as feedstocks based on previous sugar release analysis. We investigated compositional analysis and physicochemical characterizations of these poplars were performed and the correlations between these physicochemical properties and enzymatic hydrolysis yield. Gel permeation chromatography (GPC) and 13C solid state NMR were used to determine the degree of polymerization (DP) and crystallinity index (CrI) of cellulose, and the results along with the sugar release study indicated that cellulose DP likely played a more important role in enzymatic hydrolysis. Simons' stain revealed that the accessible surface area of substrate significantly varied among these variants from 17.3 to 33.2 mg g$-1\atop{biomass}$ as reflected by dye adsorption, and cellulose accessibility was shown as one of the major factors governing substrates digestibility. Furthermore, HSQC and 31P NMR analysis detailed the structural features of poplar lignin variants. Overall, cellulose relevant factors appeared to have a stronger correlation with glucose release, if any, than lignin structural features. Lignin structural features, such as a phenolic hydroxyl group and the ratio of syringyl and guaiacyl (S/G), were found to have a more convincing impact on xylose release. Low lignin content, low cellulose DP, and high cellulose accessibility generally favor enzymatic hydrolysis; however, recalcitrance cannot be simply judged on any single substrate factor.},
doi = {10.1002/cssc.201601303},
journal = {ChemSusChem},
number = 1,
volume = 10,
place = {United States},
year = {2016},
month = {11}
}

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Works referenced in this record:

Substrate and Enzyme Characteristics that Limit Cellulose Hydrolysis
journal, October 1999

  • Mansfield, S. D.; Mooney, C.; Saddler, J. N.
  • Biotechnology Progress, Vol. 15, Issue 5
  • DOI: 10.1021/bp9900864

Sodium hydroxide pretreatment and enzymatic hydrolysis of coastal Bermuda grass
journal, May 2010


The characterization of pretreated lignocellulosic substrates prior to enzymatic hydrolysis, part 1: A modified Simons' staining technique
journal, September 2008

  • Chandra, Richard; Ewanick, Shannon; Hsieh, Carmen
  • Biotechnology Progress, Vol. 24, Issue 5
  • DOI: 10.1002/btpr.33

Assessing the molecular structure basis for biomass recalcitrance during dilute acid and hydrothermal pretreatments
journal, January 2013


Characterization and analysis of the molecular weight of lignin for biorefining studies
journal, June 2014

  • Tolbert, Allison; Akinosho, Hannah; Khunsupat, Ratayakorn
  • Biofuels, Bioproducts and Biorefining, Vol. 8, Issue 6
  • DOI: 10.1002/bbb.1500

Application of quantitative 31P NMR in biomass lignin and biofuel precursors characterization
journal, January 2011

  • Pu, Yunqiao; Cao, Shilin; Ragauskas, Arthur J.
  • Energy & Environmental Science, Vol. 4, Issue 9
  • DOI: 10.1039/c1ee01201k

Physicochemical Structural Changes of Poplar and Switchgrass during Biomass Pretreatment and Enzymatic Hydrolysis
journal, July 2016


Lignin content in natural Populus variants affects sugar release
journal, March 2011

  • Studer, M. H.; DeMartini, J. D.; Davis, M. F.
  • Proceedings of the National Academy of Sciences, Vol. 108, Issue 15, p. 6300-6305
  • DOI: 10.1073/pnas.1009252108

Pretreatment and Lignocellulosic Chemistry
journal, May 2012


Structural Characterization of Lignin in Wild-Type versus COMT Down-Regulated Switchgrass
journal, January 2014


Microbial Cellulose Utilization: Fundamentals and Biotechnology
journal, September 2002

  • Lynd, L. R.; Weimer, P. J.; van Zyl, W. H.
  • Microbiology and Molecular Biology Reviews, Vol. 66, Issue 3, p. 506-577
  • DOI: 10.1128/MMBR.66.3.506-577.2002

Effects of drying-induced fiber hornification on enzymatic saccharification of lignocelluloses
journal, January 2011


Effect of Lignin Chemistry on the Enzymatic Hydrolysis of Woody Biomass
journal, June 2014


Analyzing cellulose degree of polymerization and its relevancy to cellulosic ethanol
journal, January 2011

  • Hallac, Bassem B.; Ragauskas, Arthur J.
  • Biofuels, Bioproducts and Biorefining, Vol. 5, Issue 2
  • DOI: 10.1002/bbb.269

Effects of wet-pressing-induced fiber hornification on enzymatic saccharification of lignocelluloses
journal, April 2011


Antisense Down-Regulation of 4CL Expression Alters Lignification, Tree Growth, and Saccharification Potential of Field-Grown Poplar
journal, August 2010

  • Voelker, Steven L.; Lachenbruch, Barbara; Meinzer, Frederick C.
  • Plant Physiology, Vol. 154, Issue 2
  • DOI: 10.1104/pp.110.159269

Theory, practice and prospects of X-ray and neutron scattering for lignocellulosic biomass characterization: towards understanding biomass pretreatment
journal, January 2015

  • Cheng, Gang; Zhang, Xin; Simmons, Blake
  • Energy & Environmental Science, Vol. 8, Issue 2
  • DOI: 10.1039/C4EE03147D

Genomics of cellulosic biofuels
journal, August 2008


Biomass Characterization: Recent Progress in Understanding Biomass Recalcitrance
journal, August 2012

  • Foston, Marcus; Ragauskas, Arthur J.
  • Industrial Biotechnology, Vol. 8, Issue 4
  • DOI: 10.1089/ind.2012.0015

Helically agitated mixing in dry dilute acid pretreatment enhances the bioconversion of corn stover into ethanol
journal, January 2014

  • He, Yanqing; Zhang, Longping; Zhang, Jian
  • Biotechnology for Biofuels, Vol. 7, Issue 1
  • DOI: 10.1186/1754-6834-7-1

Structural Transformation of Isolated Poplar and Switchgrass Lignins during Dilute Acid Treatment
journal, August 2015


Biomass Recalcitrance: Engineering Plants and Enzymes for Biofuels Production
journal, February 2007

  • Himmel, M. E.; Ding, S.-Y.; Johnson, D. K.
  • Science, Vol. 315, Issue 5813, p. 804-807
  • DOI: 10.1126/science.1137016

Recent advances in understanding the role of cellulose accessibility in enzymatic hydrolysis of lignocellulosic substrates
journal, June 2014


Cellulose crystallinity - a key predictor of the enzymatic hydrolysis rate: Cellulose crystallinity
journal, February 2010


Porosity and Its Effect on the Digestibility of Dilute Sulfuric Acid Pretreated Corn Stover
journal, April 2007

  • Ishizawa, Claudia I.; Davis, Mark F.; Schell, Daniel F.
  • Journal of Agricultural and Food Chemistry, Vol. 55, Issue 7
  • DOI: 10.1021/jf062131a

Inhibition of cellulase, xylanase and β-glucosidase activities by softwood lignin preparations
journal, September 2006


The Path Forward for Biofuels and Biomaterials
journal, January 2006

  • Ragauskas, Arthur J.; Williams, Charlotte K.; Davison, Brian H.
  • Science, Vol. 311, Issue 5760, p. 484-489
  • DOI: 10.1126/science.1114736

The effect of initial pore volume and lignin content on the enzymatic hydrolysis of softwoods
journal, May 1998

  • Mooney, Caitriona A.; Mansfield, Shawn D.; Touhy, Maria G.
  • Bioresource Technology, Vol. 64, Issue 2, p. 113-119
  • DOI: 10.1016/S0960-8524(97)00181-8

Substrate-Related Factors Affecting Enzymatic Saccharification of Lignocelluloses: Our Recent Understanding
journal, November 2012


High-resolution genetic mapping of allelic variants associated with cell wall chemistry in Populus
journal, January 2015


Increase in 4-Coumaryl Alcohol Units during Lignification in Alfalfa ( Medicago sativa ) Alters the Extractability and Molecular Weight of Lignin
journal, October 2010

  • Ziebell, Angela; Gracom, Kristen; Katahira, Rui
  • Journal of Biological Chemistry, Vol. 285, Issue 50
  • DOI: 10.1074/jbc.M110.137315

Changes in lignocellulosic supramolecular and ultrastructure during dilute acid pretreatment of Populus and switchgrass
journal, December 2010


Comparison Study on the Biomass Recalcitrance of Different Tissue Fractions of Sugarcane Culm
journal, June 2014


Investigating plant cell wall components that affect biomass recalcitrance in poplar and switchgrass
journal, January 2013

  • DeMartini, Jaclyn D.; Pattathil, Sivakumar; Miller, Jeffrey S.
  • Energy & Environmental Science, Vol. 6, Issue 3
  • DOI: 10.1039/c3ee23801f

Techno-economic evaluation of integrated first- and second-generation ethanol production from grain and straw
journal, January 2016

  • Joelsson, Elisabeth; Erdei, Borbála; Galbe, Mats
  • Biotechnology for Biofuels, Vol. 9, Issue 1
  • DOI: 10.1186/s13068-015-0423-8

Effect of structural and physico-chemical features of cellulosic substrates on the efficiency of enzymatic hydrolysis
journal, July 1991

  • Sinitsyn, A. P.; Gusakov, A. V.; Vlasenko, E. Yu.
  • Applied Biochemistry and Biotechnology, Vol. 30, Issue 1
  • DOI: 10.1007/BF02922023

Cellulose Isolation Methodology for NMR Analysis of Cellulose Ultrastructure
journal, November 2011

  • Foston, Marcus B.; Hubbell, Chistopher A.; Ragauskas, Art J.
  • Materials, Vol. 4, Issue 11
  • DOI: 10.3390/ma4111985

Role of Functional Groups in Lignin Inhibition of Enzymatic Hydrolysis of Cellulose to Glucose
journal, March 2008


Toward an aggregated understanding of enzymatic hydrolysis of cellulose: Noncomplexed cellulase systems
journal, November 2004

  • Zhang, Yi-Heng Percival; Lynd, Lee R.
  • Biotechnology and Bioengineering, Vol. 88, Issue 7, p. 797-824
  • DOI: 10.1002/bit.20282

Variation of S/G Ratio and Lignin Content in a <i>Populus</i> Family Influences the Release of Xylose by Dilute Acid Hydrolysis
journal, January 2006

  • Davison, Brian H.; Drescher, Sadie R.; Tuskan, Gerald A.
  • Applied Biochemistry and Biotechnology, Vol. 130, Issue 1-3
  • DOI: 10.1385/ABAB:130:1:427

Determination of porosity of lignocellulosic biomass before and after pretreatment by using Simons’ stain and NMR techniques
journal, September 2013


Enhancing the enzymatic hydrolysis of lignocellulosic biomass by increasing the carboxylic acid content of the associated lignin
journal, November 2010

  • Nakagame, Seiji; Chandra, Richard P.; Kadla, John F.
  • Biotechnology and Bioengineering, Vol. 108, Issue 3
  • DOI: 10.1002/bit.22981

    Works referencing / citing this record:

    Lignocellulosic Biomass: Understanding Recalcitrance and Predicting Hydrolysis
    journal, December 2019