skip to main content
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Topochemical Understanding of Lignin Distribution During Hydrothermal Flowthrough Pretreatment

Abstract

Changes in surface properties during biomass pretreatments are important parameters to understand and engineer biological biomass conversion processes. In particular, different influences on the surface of biomass are expected between flowthrough and batch pretreatments. In this paper, for a better understanding of biomass surface changes by hydrothermal flowthrough pretreatment, the mechanism by which the surface of biomass is altered in terms of cellulose and lignin was investigated using time-of-flight secondary ion mass spectrometry (ToF-SIMS) and compared with the bulk chemical composition and the results from scanning electron microscope (SEM). ToF-SIMS analysis results provide semi-quantitative information of cellulose and lignin and support the other observation from SEM and bulk compositional analyses. In brief, more lignin was observed on the surface of biomass at the early stage hydrothermal pretreatment, while the lignin mainly located at the cell corners was reduced by extended pretreatment time. Finally, unlike batch pretreatment, pseudo-lignin formation was not observed on the poplar surface during the flowthrough process.

Authors:
 [1];  [2];  [3];  [4];  [1];  [1];  [5]; ORCiD logo [6]
  1. 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. Center for Bioenergy Innovation
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). BioEnergy Science Center. Center for Bioenergy Innovation; Univ. of California, Riverside, CA (United States). Dept. of Chemical & Environmental Engineering. Center for Environmental Research and Technology; Univ. of British Columbia, Vancouver, BC (Canada). Dept. of Chemical and Biological Engineering
  3. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). BioEnergy Science Center. Center for Bioenergy Innovation. UT-ORNL Joint Inst. for Biological Science
  4. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). BioEnergy Science Center. Center for Bioenergy Innovation; Washington Univ., St. Louis, MO (United States). Dept. of Energy, Environmental & Chemical Engineering
  5. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). BioEnergy Science Center. Center for Bioenergy Innovation; Univ. of California, Riverside, CA (United States). Dept. of Chemical & Environmental Engineering. Center for Environmental Research and Technology
  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. Center for Bioenergy Innovation. UT-ORNL Joint Inst. for Biological Science; Univ. of Tennessee, Knoxville, TN (United States). Dept. of Chemical and Biomolecular Engineering. Dept. of Forestry, Wildlife, Fisheries
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Biological and Environmental Research (BER) (SC-23)
OSTI Identifier:
1468139
Grant/Contract Number:  
[AC05-00OR22725]
Resource Type:
Accepted Manuscript
Journal Name:
Chemistry Select
Additional Journal Information:
[ Journal Volume: 3; Journal Issue: 32]; Journal ID: ISSN 2365-6549
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; flowthrough pretreatment; surface characteristics; ToF-SIMS; topochemical effect

Citation Formats

Jung, Seokwon, Trajano, Heather L., Yoo, Chang Geun, Foston, Marcus B., Hu, Fan, Tolbert, Allison K., Wyman, Charles E., and Ragauskas, Arthur J. Topochemical Understanding of Lignin Distribution During Hydrothermal Flowthrough Pretreatment. United States: N. p., 2018. Web. doi:10.1002/slct.201801837.
Jung, Seokwon, Trajano, Heather L., Yoo, Chang Geun, Foston, Marcus B., Hu, Fan, Tolbert, Allison K., Wyman, Charles E., & Ragauskas, Arthur J. Topochemical Understanding of Lignin Distribution During Hydrothermal Flowthrough Pretreatment. United States. doi:10.1002/slct.201801837.
Jung, Seokwon, Trajano, Heather L., Yoo, Chang Geun, Foston, Marcus B., Hu, Fan, Tolbert, Allison K., Wyman, Charles E., and Ragauskas, Arthur J. Mon . "Topochemical Understanding of Lignin Distribution During Hydrothermal Flowthrough Pretreatment". United States. doi:10.1002/slct.201801837. https://www.osti.gov/servlets/purl/1468139.
@article{osti_1468139,
title = {Topochemical Understanding of Lignin Distribution During Hydrothermal Flowthrough Pretreatment},
author = {Jung, Seokwon and Trajano, Heather L. and Yoo, Chang Geun and Foston, Marcus B. and Hu, Fan and Tolbert, Allison K. and Wyman, Charles E. and Ragauskas, Arthur J.},
abstractNote = {Changes in surface properties during biomass pretreatments are important parameters to understand and engineer biological biomass conversion processes. In particular, different influences on the surface of biomass are expected between flowthrough and batch pretreatments. In this paper, for a better understanding of biomass surface changes by hydrothermal flowthrough pretreatment, the mechanism by which the surface of biomass is altered in terms of cellulose and lignin was investigated using time-of-flight secondary ion mass spectrometry (ToF-SIMS) and compared with the bulk chemical composition and the results from scanning electron microscope (SEM). ToF-SIMS analysis results provide semi-quantitative information of cellulose and lignin and support the other observation from SEM and bulk compositional analyses. In brief, more lignin was observed on the surface of biomass at the early stage hydrothermal pretreatment, while the lignin mainly located at the cell corners was reduced by extended pretreatment time. Finally, unlike batch pretreatment, pseudo-lignin formation was not observed on the poplar surface during the flowthrough process.},
doi = {10.1002/slct.201801837},
journal = {Chemistry Select},
number = [32],
volume = [3],
place = {United States},
year = {2018},
month = {8}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Citation Metrics:
Cited by: 1 work
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

Chemical transformations of Populus trichocarpa during dilute acid pretreatment
journal, January 2012

  • Cao, Shilin; Pu, Yunqiao; Studer, Michael
  • RSC Advances, Vol. 2, Issue 29
  • DOI: 10.1039/c2ra22045h

The hydrothermal degradation of cellulosic matter to sugars and their fermentative conversion to protein
journal, August 1976


Topochemical pretreatment of wood biomass to enhance enzymatic hydrolysis of polysaccharides to sugars
journal, August 2013


Advances in understanding the surface chemistry of lignocellulosic biomass via time-of-flight secondary ion mass spectrometry
journal, December 2016

  • Tolbert, Allison; Ragauskas, Arthur J.
  • Energy Science & Engineering, Vol. 5, Issue 1
  • DOI: 10.1002/ese3.144

Current Understanding of the Correlation of Lignin Structure with Biomass Recalcitrance
journal, November 2016


Lignin plays a negative role in the biochemical process for producing lignocellulosic biofuels
journal, June 2014


Visualizing lignin coalescence and migration through maize cell walls following thermochemical pretreatment
journal, December 2008

  • Donohoe, Bryon S.; Decker, Stephen R.; Tucker, Melvin P.
  • Biotechnology and Bioengineering, Vol. 101, Issue 5
  • DOI: 10.1002/bit.21959

Pseudo-lignin and pretreatment chemistry
journal, January 2011

  • Sannigrahi, Poulomi; Kim, Dong Ho; Jung, Seokwon
  • Energy Environ. Sci., Vol. 4, Issue 4
  • DOI: 10.1039/C0EE00378F

Identifying the Characteristic Secondary Ions of Lignin Polymer Using ToF−SIMS
journal, March 2005

  • Saito, Kaori; Kato, Toshiyuki; Tsuji, Yukiko
  • Biomacromolecules, Vol. 6, Issue 2
  • DOI: 10.1021/bm049521v

The fate of lignin during hydrothermal pretreatment
journal, January 2013

  • Trajano, Heather L.; Engle, Nancy L.; Foston, Marcus
  • Biotechnology for Biofuels, Vol. 6, Issue 1
  • DOI: 10.1186/1754-6834-6-110

The Effect of Flow Rate of Compressed Hot Water on Xylan, Lignin, and Total Mass Removal from Corn Stover
journal, September 2003

  • Liu, Chaogang; Wyman, Charles E.
  • Industrial & Engineering Chemistry Research, Vol. 42, Issue 21, p. 5409-5416
  • DOI: 10.1021/ie030458k

Modification of fibre surfaces during pulping and refining as analysed by SEM, XPS and ToF-SIMS
journal, August 2003

  • Fardim, Pedro; Durán, Nelson
  • Colloids and Surfaces A: Physicochemical and Engineering Aspects, Vol. 223, Issue 1-3
  • DOI: 10.1016/S0927-7757(03)00149-3

Extractives on fiber surfaces investigated by XPS, ToF-SIMS and AFM
journal, March 2005

  • Fardim, Pedro; Gustafsson, Johanna; von Schoultz, Sebastian
  • Colloids and Surfaces A: Physicochemical and Engineering Aspects, Vol. 255, Issue 1-3
  • DOI: 10.1016/j.colsurfa.2004.12.027

Surface and ultrastructural characterization of raw and pretreated switchgrass
journal, December 2011


Features of promising technologies for pretreatment of lignocellulosic biomass
journal, April 2005


Xylan hydrolysis in Populus trichocarpa×P. deltoides and model substrates during hydrothermal pretreatment
journal, March 2015


Structural Characterization and Comparison of Switchgrass Ball-milled Lignin Before and After Dilute Acid Pretreatment
journal, August 2009

  • Samuel, Reichel; Pu, Yunqiao; Raman, Babu
  • Applied Biochemistry and Biotechnology, Vol. 162, Issue 1
  • DOI: 10.1007/s12010-009-8749-y

Flowthrough pretreatment with very dilute acid provides insights into high lignin contribution to biomass recalcitrance
journal, November 2016


Effect of xylan and lignin removal by batch and flowthrough pretreatment on the enzymatic digestibility of corn stover cellulose
journal, January 2004

  • Yang, Bin; Wyman, Charles E.
  • Biotechnology and Bioengineering, Vol. 86, Issue 1
  • DOI: 10.1002/bit.20043

3D Chemical Image using TOF-SIMS Revealing the Biopolymer Component Spatial and Lateral Distributions in Biomass
journal, October 2012

  • Jung, Seokwon; Foston, Marcus; Kalluri, Udaya C.
  • Angewandte Chemie, Vol. 124, Issue 48
  • DOI: 10.1002/ange.201205243