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Title: Hemicellulose–Cellulose Composites Reveal Differences in Cellulose Organization after Dilute Acid Pretreatment

Abstract

Model hemicellulose–cellulose composites that mimic plant cell wall polymer interactions were prepared by synthesizing deuterated bacterial cellulose in the presence of glucomannan or xyloglucan. Dilute acid pretreatment (DAP) of these materials was studied using small-angle neutron scattering, X-ray diffraction, and sum frequency generation spectroscopy. The macrofibril dimensions of the pretreated cellulose alone were smaller but with similar entanglement of macrofibrillar network as native cellulose. In addition, the crystallite size dimension along the (010) plane increased. Glucomannan–cellulose underwent similar changes to cellulose, except that the macrofibrillar network was more entangled after DAP. Conversely, in xyloglucan–cellulose the macrofibril dimensions and macrofibrillar network were relatively unchanged after pretreatment, but the cellulose Iβ content was increased. Our results point to a tight interaction of xyloglucan with microfibrils while glucomannan only interacts with macrofibril surfaces. Furthermore, this study provides insight into roles of different hemicellulose–cellulose interactions and may help in improving pretreatment processes or engineering plants with decreased recalcitrance.

Authors:
 [1];  [2]; ORCiD logo [3]; ORCiD logo [3]; ORCiD logo [3]; ORCiD logo [3]; ORCiD logo [3]; ORCiD logo [2]; ORCiD logo [3]; ORCiD logo [3]; ORCiD logo [3]
  1. Univ. of Tennessee, Knoxville, TN (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  2. Pennsylvania State Univ., State College, PA (United States)
  3. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Center for Lignocellulose Structure and Formation (CLSF); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Biological and Environmental Research (BER); USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1506814
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Biomacromolecules
Additional Journal Information:
Journal Volume: 20; Journal Issue: 2; Journal ID: ISSN 1525-7797
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
59 BASIC BIOLOGICAL SCIENCES

Citation Formats

Shah, Riddhi S., Huang, Shixin, Pingali, Sai Venkatesh, Sawada, Daisuke, Pu, Yunqiao, Rodriguez, Jr., Miguel, Ragauskas, Arthur J., Kim, Seong H., Evans, Barbara R., Davison, II, Brian H., and O’Neill, Hugh. Hemicellulose–Cellulose Composites Reveal Differences in Cellulose Organization after Dilute Acid Pretreatment. United States: N. p., 2018. Web. doi:10.1021/acs.biomac.8b01511.
Shah, Riddhi S., Huang, Shixin, Pingali, Sai Venkatesh, Sawada, Daisuke, Pu, Yunqiao, Rodriguez, Jr., Miguel, Ragauskas, Arthur J., Kim, Seong H., Evans, Barbara R., Davison, II, Brian H., & O’Neill, Hugh. Hemicellulose–Cellulose Composites Reveal Differences in Cellulose Organization after Dilute Acid Pretreatment. United States. https://doi.org/10.1021/acs.biomac.8b01511
Shah, Riddhi S., Huang, Shixin, Pingali, Sai Venkatesh, Sawada, Daisuke, Pu, Yunqiao, Rodriguez, Jr., Miguel, Ragauskas, Arthur J., Kim, Seong H., Evans, Barbara R., Davison, II, Brian H., and O’Neill, Hugh. 2018. "Hemicellulose–Cellulose Composites Reveal Differences in Cellulose Organization after Dilute Acid Pretreatment". United States. https://doi.org/10.1021/acs.biomac.8b01511. https://www.osti.gov/servlets/purl/1506814.
@article{osti_1506814,
title = {Hemicellulose–Cellulose Composites Reveal Differences in Cellulose Organization after Dilute Acid Pretreatment},
author = {Shah, Riddhi S. and Huang, Shixin and Pingali, Sai Venkatesh and Sawada, Daisuke and Pu, Yunqiao and Rodriguez, Jr., Miguel and Ragauskas, Arthur J. and Kim, Seong H. and Evans, Barbara R. and Davison, II, Brian H. and O’Neill, Hugh},
abstractNote = {Model hemicellulose–cellulose composites that mimic plant cell wall polymer interactions were prepared by synthesizing deuterated bacterial cellulose in the presence of glucomannan or xyloglucan. Dilute acid pretreatment (DAP) of these materials was studied using small-angle neutron scattering, X-ray diffraction, and sum frequency generation spectroscopy. The macrofibril dimensions of the pretreated cellulose alone were smaller but with similar entanglement of macrofibrillar network as native cellulose. In addition, the crystallite size dimension along the (010) plane increased. Glucomannan–cellulose underwent similar changes to cellulose, except that the macrofibrillar network was more entangled after DAP. Conversely, in xyloglucan–cellulose the macrofibril dimensions and macrofibrillar network were relatively unchanged after pretreatment, but the cellulose Iβ content was increased. Our results point to a tight interaction of xyloglucan with microfibrils while glucomannan only interacts with macrofibril surfaces. Furthermore, this study provides insight into roles of different hemicellulose–cellulose interactions and may help in improving pretreatment processes or engineering plants with decreased recalcitrance.},
doi = {10.1021/acs.biomac.8b01511},
url = {https://www.osti.gov/biblio/1506814}, journal = {Biomacromolecules},
issn = {1525-7797},
number = 2,
volume = 20,
place = {United States},
year = {Mon Dec 17 00:00:00 EST 2018},
month = {Mon Dec 17 00:00:00 EST 2018}
}

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