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

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.

doi:10.1039/C7GC03518G

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

Journal Article · Tue Jan 23 00:00:00 EST 2018 · Green Chemistry

DOI:https://doi.org/10.1039/C7GC03518G· OSTI ID:1474556

^[1]; Bhagia, Samarthya ^[2];

^[3]; Petridis, Loukas ^[3]; Ong, Rebecca G. ^[4];

^[5]; Mittal, Ashutosh ^[6]; Himmel, Michael H. ^[7];

^[8];

^[9];

^[10]; Smith, Jeremy C. ^[11]; Wyman, Charles E. ^[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). 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
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
Michigan Technological Univ., Houghton, MI (United States). Dept. of Chemical Engineering, DOE Great Lakes Bioenergy Research Center (GLBRC)
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
National Renewable Energy Lab. (NREL), Golden, CO (United States). Biosciences Center
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
Univ. of Houston, Houston, TX (United States). Dept. of Engineering Technology, Biotechnology Division, School of Technology
Michigan State Univ., East Lansing, MI (United States). Dept. of Chemical Engineering and Materials Science, DOE Great Lakes Bioenergy Research Center (GLBRC)
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
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
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

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.

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Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Oak Ridge Leadership Computing Facility (OLCF)

Sponsoring Organization:: USDOE Office of Science (SC), Biological and Environmental Research (BER)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1474556

Journal Information:: Green Chemistry, Vol. 20, Issue 4; ISSN 1463-9262

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 37 works

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