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Title: Cellulose–hemicellulose interactions at elevated temperatures increase cellulose recalcitrance to biological conversion

It has been previously shown that cellulose-lignin droplets’ strong interactions, resulting from lignin coalescence and redisposition on cellulose surface during thermochemical pretreatments, increase cellulose recalcitrance to biological conversion, especially at commercially viable low enzyme loadings. However, information on the impact of cellulose–hemicellulose interactions on cellulose recalcitrance following relevant pretreatment conditions are scarce. Here, to investigate the effects of plausible hemicellulose precipitation and re-association with cellulose on cellulose conversion, different pretreatments were applied to pure Avicel® PH101 cellulose alone and Avicel mixed with model hemicellulose compounds followed by enzymatic hydrolysis of resulting solids at both low and high enzyme loadings. Solids produced by pretreatment of Avicel mixed with hemicelluloses (AMH) were found to contain about 2 to 14.6% of exogenous, precipitated hemicelluloses and showed a remarkably much lower digestibility (up to 60%) than their respective controls. However, the exogenous hemicellulosic residues that associated with Avicel following high temperature pretreatments resulted in greater losses in cellulose conversion than those formed at low temperatures, suggesting that temperature plays a strong role in the strength of cellulose–hemicellulose association. Molecular dynamics simulations of hemicellulosic xylan and cellulose were found to further support this temperature effect as the xylan–cellulose interactions were found to substantially increase atmore » elevated temperatures. Furthermore, exogenous, precipitated hemicelluloses in pretreated AMH solids resulted in a larger drop in cellulose conversion than the delignified lignocellulosic biomass containing comparably much higher natural hemicellulose amounts. In conclusion, increased cellulase loadings or supplementation of cellulase with xylanases enhanced cellulose conversion for most pretreated AMH solids; however, this approach was less effective for solids containing mannan polysaccharides, suggesting stronger association of cellulose with (hetero) mannans or lack of enzymes in the mixture required to hydrolyze such polysaccharides.« less
Authors:
ORCiD logo [1] ;  [2] ; ORCiD logo [3] ;  [3] ;  [4] ; ORCiD logo [5] ;  [6] ;  [7] ; ORCiD logo [8] ; ORCiD logo [9] ; ORCiD logo [10] ;  [11] ;  [12]
  1. Univ. of California, Riverside, CA (United States). Center for Environmental Research and Technology (CE-CERT), Bourns College of Engineering; Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). BioEnergy Science Center (BESC); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Bioenergy Innovation (CBI)
  2. Univ. of California, Riverside, CA (United States). Center for Environmental Research and Technology (CE-CERT), Bourns College of Engineering; Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). BioEnergy Science Center (BESC); Univ. of California, Riverside, CA (United States). Dept. of Chemical and Environmental Engineering, Bourns College of Engineering; Univ. of Tennessee, Knoxville, TN (United States). Dept. of Chemical and Biomolecular Engineering
  3. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). UT/ORNL Center for Molecular Biophysics; Univ. of Tennessee, Knoxville, TN (United States). Dept. of Biochemistry, Cellular & Molecular Biology
  4. Michigan Technological Univ., Houghton, MI (United States). Dept. of Chemical Engineering, DOE Great Lakes Bioenergy Research Center (GLBRC)
  5. Univ. of California, Riverside, CA (United States). Center for Environmental Research and Technology (CE-CERT), Bourns College of Engineering; Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Bioenergy Innovation (CBI); Univ. of California, Riverside, CA (United States). Dept. of Chemical and Environmental Engineering, Bourns College of Engineering
  6. National Renewable Energy Lab. (NREL), Golden, CO (United States). Biosciences Center
  7. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). BioEnergy Science Center (BESC); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Bioenergy Innovation (CBI); National Renewable Energy Lab. (NREL), Golden, CO (United States). Biosciences Center
  8. Univ. of Houston, Houston, TX (United States). Dept. of Engineering Technology, Biotechnology Division, School of Technology
  9. Michigan State Univ., East Lansing, MI (United States). Dept. of Chemical Engineering and Materials Science, DOE Great Lakes Bioenergy Research Center (GLBRC)
  10. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). BioEnergy Science Center (BESC); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Bioenergy Innovation (CBI); Univ. of Tennessee, Knoxville, TN (United States). Dept. of Chemical and Biomolecular Engineering; Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Joint Inst. of Biological Sciences, Biosciences Division; Univ. of Tennessee, Knoxville, TN (United States). Center for Renewable Carbon, Dept. of Forestry, Wildlife, and Fisheries
  11. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). BioEnergy Science Center (BESC); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). UT/ORNL Center for Molecular Biophysics; Univ. of Tennessee, Knoxville, TN (United States). Dept. of Biochemistry, Cellular & Molecular Biology
  12. Univ. of California, Riverside, CA (United States). Center for Environmental Research and Technology (CE-CERT), Bourns College of Engineering; Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). BioEnergy Science Center (BESC); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Bioenergy Innovation (CBI); Univ. of California, Riverside, CA (United States). Dept. of Chemical and Environmental Engineering, Bourns College of Engineering
Publication Date:
Grant/Contract Number:
AC05-00OR22725
Type:
Accepted Manuscript
Journal Name:
Green Chemistry
Additional Journal Information:
Journal Volume: 20; Journal Issue: 4; Journal ID: ISSN 1463-9262
Publisher:
Royal Society of Chemistry
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)
Country of Publication:
United States
Language:
English
Subject:
59 BASIC BIOLOGICAL SCIENCES
OSTI Identifier:
1474556

Kumar, Rajeev, Bhagia, Samarthya, Smith, Micholas Dean, Petridis, Loukas, Ong, Rebecca G., Cai, Charles M., Mittal, Ashutosh, Himmel, Michael H., Balan, Venkatesh, Dale, Bruce E., Ragauskas, Arthur J., Smith, Jeremy C., and Wyman, Charles E.. Cellulose–hemicellulose interactions at elevated temperatures increase cellulose recalcitrance to biological conversion. United States: N. p., Web. doi:10.1039/C7GC03518G.
Kumar, Rajeev, Bhagia, Samarthya, Smith, Micholas Dean, Petridis, Loukas, Ong, Rebecca G., Cai, Charles M., Mittal, Ashutosh, Himmel, Michael H., Balan, Venkatesh, Dale, Bruce E., Ragauskas, Arthur J., Smith, Jeremy C., & Wyman, Charles E.. Cellulose–hemicellulose interactions at elevated temperatures increase cellulose recalcitrance to biological conversion. United States. doi:10.1039/C7GC03518G.
Kumar, Rajeev, Bhagia, Samarthya, Smith, Micholas Dean, Petridis, Loukas, Ong, Rebecca G., Cai, Charles M., Mittal, Ashutosh, Himmel, Michael H., Balan, Venkatesh, Dale, Bruce E., Ragauskas, Arthur J., Smith, Jeremy C., and Wyman, Charles E.. 2018. "Cellulose–hemicellulose interactions at elevated temperatures increase cellulose recalcitrance to biological conversion". United States. doi:10.1039/C7GC03518G.
@article{osti_1474556,
title = {Cellulose–hemicellulose interactions at elevated temperatures increase cellulose recalcitrance to biological conversion},
author = {Kumar, Rajeev and Bhagia, Samarthya and Smith, Micholas Dean and Petridis, Loukas and Ong, Rebecca G. and Cai, Charles M. and Mittal, Ashutosh and Himmel, Michael H. and Balan, Venkatesh and Dale, Bruce E. and Ragauskas, Arthur J. and Smith, Jeremy C. and Wyman, Charles E.},
abstractNote = {It has been previously shown that cellulose-lignin droplets’ strong interactions, resulting from lignin coalescence and redisposition on cellulose surface during thermochemical pretreatments, increase cellulose recalcitrance to biological conversion, especially at commercially viable low enzyme loadings. However, information on the impact of cellulose–hemicellulose interactions on cellulose recalcitrance following relevant pretreatment conditions are scarce. Here, to investigate the effects of plausible hemicellulose precipitation and re-association with cellulose on cellulose conversion, different pretreatments were applied to pure Avicel® PH101 cellulose alone and Avicel mixed with model hemicellulose compounds followed by enzymatic hydrolysis of resulting solids at both low and high enzyme loadings. Solids produced by pretreatment of Avicel mixed with hemicelluloses (AMH) were found to contain about 2 to 14.6% of exogenous, precipitated hemicelluloses and showed a remarkably much lower digestibility (up to 60%) than their respective controls. However, the exogenous hemicellulosic residues that associated with Avicel following high temperature pretreatments resulted in greater losses in cellulose conversion than those formed at low temperatures, suggesting that temperature plays a strong role in the strength of cellulose–hemicellulose association. Molecular dynamics simulations of hemicellulosic xylan and cellulose were found to further support this temperature effect as the xylan–cellulose interactions were found to substantially increase at elevated temperatures. Furthermore, exogenous, precipitated hemicelluloses in pretreated AMH solids resulted in a larger drop in cellulose conversion than the delignified lignocellulosic biomass containing comparably much higher natural hemicellulose amounts. In conclusion, increased cellulase loadings or supplementation of cellulase with xylanases enhanced cellulose conversion for most pretreated AMH solids; however, this approach was less effective for solids containing mannan polysaccharides, suggesting stronger association of cellulose with (hetero) mannans or lack of enzymes in the mixture required to hydrolyze such polysaccharides.},
doi = {10.1039/C7GC03518G},
journal = {Green Chemistry},
number = 4,
volume = 20,
place = {United States},
year = {2018},
month = {1}
}

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