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Title: Effect of lignin content on changes occurring in poplar cellulose ultrastructure during dilute acid pretreatment

Journal Article · · Biotechnology for Biofuels
 [1];  [2];  [1];  [3];  [3];  [3];  [4];  [5];  [3];  [6];  [5]
  1. Georgia Inst. of Technology, Atlanta, GA (United States). School of Chemistry and Biochemistry
  2. Washington Univ., St. Louis, MO (United States)
  3. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Structural Molecular Biology (CSMB)
  4. Univ. of California, Riverside, CA (United States). Bourns College of Engineering
  5. Univ. of California, Riverside, CA (United States). Bourns College of Engineering; Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). BioEnergy Science Center (BESC)
  6. Georgia Inst. of Technology, Atlanta, GA (United States). School of Chemistry and Biochemistry; Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). BioEnergy Science Center (BESC); Univ. of Tennessee, Knoxville, TN (United States)

Obtaining a better understanding of the complex mechanisms occurring during lignocellulosic deconstruction is critical to the continued growth of renewable biofuel production. A key step in bioethanol production is thermochemical pretreatment to reduce plant cell wall recalcitrance for downstream processes. Previous studies of dilute acid pretreatment (DAP) have shown significant changes in cellulose ultrastructure that occur during pretreatment, but there is still a substantial knowledge gap with respect to the influence of lignin on these cellulose ultrastructural changes. This study was designed to assess how the presence of lignin influences DAP-induced changes in cellulose ultrastructure, which might ultimately have large implications with respect to enzymatic deconstruction efforts. Native, untreated hybrid poplar (Populus trichocarpa x Populus deltoids) samples and a partially delignified poplar sample (facilitated by acidic sodium chlorite pulping) were separately pretreated with dilute sulfuric acid (0.10 M) at 160°C for 15 minutes and 35 minutes, respectively . Following extensive characterization, the partially delignified biomass displayed more significant changes in cellulose ultrastructure following DAP than the native untreated biomass. With respect to the native untreated poplar, delignified poplar after DAP (in which approximately 40% lignin removal occurred) experienced: increased cellulose accessibility indicated by increased Simons’ stain (orange dye) adsorption from 21.8 to 72.5 mg/g, decreased cellulose weight-average degree of polymerization (DPw) from 3087 to 294 units, and increased cellulose crystallite size from 2.9 to 4.2 nm. These changes following DAP ultimately increased enzymatic sugar yield from 10 to 80%. We conclude that, overall, the results indicate a strong influence of lignin content on cellulose ultrastructural changes occurring during DAP. With the reduction of lignin content during DAP, the enlargement of cellulose microfibril dimensions and crystallite size becomes more apparent. Further, this enlargement of cellulose microfibril dimensions is attributed to specific processes, including the co-crystallization of crystalline cellulose driven by irreversible inter-chain hydrogen bonding (similar to hornification) and/or cellulose annealing that converts amorphous cellulose to paracrystalline and crystalline cellulose. Essentially, lignin acts as a barrier to prevent cellulose crystallinity increase and cellulose fibril coalescence during DAP.

Research Organization:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Biological and Environmental Research (BER)
Grant/Contract Number:
FWP ERKP752; FWP ERKP291
OSTI ID:
1259860
Journal Information:
Biotechnology for Biofuels, Vol. 7, Issue 1; ISSN 1754-6834
Publisher:
BioMed CentralCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 111 works
Citation information provided by
Web of Science

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Physical and chemical differences between one-stage and two-stage hydrothermal pretreated hardwood substrates for use in cellulosic ethanol production journal February 2016
Laccase mediated delignification of pineapple leaf waste: an ecofriendly sustainable attempt towards valorization journal April 2019
Production of xylooligosaccharides and monosaccharides from poplar by a two-step acetic acid and peroxide/acetic acid pretreatment journal April 2019
A study of poplar organosolv lignin after melt rheology treatment as carbon fiber precursors journal January 2016
Cellulose solvent-based pretreatment for enhanced second-generation biofuel production: a review journal January 2019
Altered lignocellulose chemical structure and molecular assembly in CINNAMYL ALCOHOL DEHYDROGENASE-deficient rice journal November 2019
Isolation and Characterization of Novel Lignolytic, Cellulolytic, and Hemicellulolytic Bacteria from Wood-Feeding Termite Cryptotermes brevis journal July 2018
Characterization of lignin derived from water-only and dilute acid flowthrough pretreatment of poplar wood at elevated temperatures journal December 2015
Advances in understanding the surface chemistry of lignocellulosic biomass via time-of-flight secondary ion mass spectrometry journal December 2016
New perspective on glycoside hydrolase binding to lignin from pretreated corn stover journal December 2015
Recent advances in understanding the pseudo-lignin formation in a lignocellulosic biorefinery journal January 2018
Saccharification of pretreated sawdust by Aspergillus niger cellulase journal March 2015