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Title: Mechanism of lignin inhibition of enzymatic biomass deconstruction

Abstract

Here, the conversion of plant biomass to ethanol via enzymatic cellulose hydrolysis offers a potentially sustainable route to biofuel production. However, the inhibition of enzymatic activity in pretreated biomass by lignin severely limits the efficiency of this process. As a result, by performing atomic-detail molecular dynamics simulation of a biomass model containing cellulose, lignin, and cellulases (TrCel7A), we elucidate detailed lignin inhibition mechanisms. We find that lignin binds preferentially both to the elements of cellulose to which the cellulases also preferentially bind (the hydrophobic faces) and also to the specific residues on the cellulose-binding module of the cellulase that are critical for cellulose binding of TrCel7A (Y466, Y492, and Y493). In conclusion, lignin thus binds exactly where for industrial purposes it is least desired, providing a simple explanation of why hydrolysis yields increase with lignin removal.

Authors:
; ; ; ; ;
Publication Date:
Research Org.:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Oak Ridge Leadership Computing Facility (OLCF)
Sponsoring Org.:
USDOE Office of Science (SC), Biological and Environmental Research (BER)
OSTI Identifier:
1618632
Alternate Identifier(s):
OSTI ID: 1260590; OSTI ID: 1327644
Grant/Contract Number:  
FWP ERKP752; AC05-00OR22725; FG02-97ER25308
Resource Type:
Journal Article: Published Article
Journal Name:
Biotechnology for Biofuels
Additional Journal Information:
Journal Name: Biotechnology for Biofuels Journal Volume: 8 Journal Issue: 1; Journal ID: ISSN 1754-6834
Publisher:
Springer Science + Business Media
Country of Publication:
Netherlands
Language:
English
Subject:
59 BASIC BIOLOGICAL SCIENCES; 09 BIOMASS FUELS; Cellulose crystallinity; Cel7A; Lignin; Biofuel; biofuel; lignin; cellulose crystallinity

Citation Formats

Vermaas, Josh V., Petridis, Loukas, Qi, Xianghong, Schulz, Roland, Lindner, Benjamin, and Smith, Jeremy. C. Mechanism of lignin inhibition of enzymatic biomass deconstruction. Netherlands: N. p., 2015. Web. doi:10.1186/s13068-015-0379-8.
Vermaas, Josh V., Petridis, Loukas, Qi, Xianghong, Schulz, Roland, Lindner, Benjamin, & Smith, Jeremy. C. Mechanism of lignin inhibition of enzymatic biomass deconstruction. Netherlands. https://doi.org/10.1186/s13068-015-0379-8
Vermaas, Josh V., Petridis, Loukas, Qi, Xianghong, Schulz, Roland, Lindner, Benjamin, and Smith, Jeremy. C. 2015. "Mechanism of lignin inhibition of enzymatic biomass deconstruction". Netherlands. https://doi.org/10.1186/s13068-015-0379-8.
@article{osti_1618632,
title = {Mechanism of lignin inhibition of enzymatic biomass deconstruction},
author = {Vermaas, Josh V. and Petridis, Loukas and Qi, Xianghong and Schulz, Roland and Lindner, Benjamin and Smith, Jeremy. C.},
abstractNote = {Here, the conversion of plant biomass to ethanol via enzymatic cellulose hydrolysis offers a potentially sustainable route to biofuel production. However, the inhibition of enzymatic activity in pretreated biomass by lignin severely limits the efficiency of this process. As a result, by performing atomic-detail molecular dynamics simulation of a biomass model containing cellulose, lignin, and cellulases (TrCel7A), we elucidate detailed lignin inhibition mechanisms. We find that lignin binds preferentially both to the elements of cellulose to which the cellulases also preferentially bind (the hydrophobic faces) and also to the specific residues on the cellulose-binding module of the cellulase that are critical for cellulose binding of TrCel7A (Y466, Y492, and Y493). In conclusion, lignin thus binds exactly where for industrial purposes it is least desired, providing a simple explanation of why hydrolysis yields increase with lignin removal.},
doi = {10.1186/s13068-015-0379-8},
url = {https://www.osti.gov/biblio/1618632}, journal = {Biotechnology for Biofuels},
issn = {1754-6834},
number = 1,
volume = 8,
place = {Netherlands},
year = {Mon Dec 21 00:00:00 EST 2015},
month = {Mon Dec 21 00:00:00 EST 2015}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record at https://doi.org/10.1186/s13068-015-0379-8

Citation Metrics:
Cited by: 153 works
Citation information provided by
Web of Science

Figures / Tables:

Fig. 1 Fig. 1: Side view of the initial state of the lignocellulosic biomass system. Cellulose fibrils are red, lignin molecules blue, and TrCel7A enzymes green; the CBMs have a lighter color than the CDs, while glycosylations and linker regions are in pastel green. An animation from this starting structure is givenmore » as an Additional file 1« less

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