Hemicellulose-Cellulose Composites Reveal Differences in Cellulose Organization after Dilute Acid Pretreatment

Riddhi Shah, Shixin Huang, Sai Venkatesh Pingali, Daisuke Sawada, Yunqiao Pu, Miguel Rodriguez, Arthur J. Ragauskas, Seong Kim, Barbara R. Evans, Brian H. Davison, Hugh O'Neill

Research output: Contribution to journalArticle

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 I β content was increased. Our results point to a tight interaction of xyloglucan with microfibrils while glucomannan only interacts with macrofibril surfaces. This study provides insight into roles of different hemicellulose-cellulose interactions and may help in improving pretreatment processes or engineering plants with decreased recalcitrance.

Original languageEnglish (US)
Pages (from-to)893-903
Number of pages11
JournalBiomacromolecules
Volume20
Issue number2
DOIs
StatePublished - Feb 11 2019

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Cellulose
Acids
Composite materials
hemicellulose
Crystallite size
Neutron scattering
Polymers
Spectroscopy
X ray diffraction
(1-6)-alpha-glucomannan
xyloglucan

All Science Journal Classification (ASJC) codes

  • Bioengineering
  • Biomaterials
  • Polymers and Plastics
  • Materials Chemistry

Cite this

Shah, R., Huang, S., Pingali, S. V., Sawada, D., Pu, Y., Rodriguez, M., ... O'Neill, H. (2019). Hemicellulose-Cellulose Composites Reveal Differences in Cellulose Organization after Dilute Acid Pretreatment. Biomacromolecules, 20(2), 893-903. https://doi.org/10.1021/acs.biomac.8b01511
Shah, Riddhi ; Huang, Shixin ; Pingali, Sai Venkatesh ; Sawada, Daisuke ; Pu, Yunqiao ; Rodriguez, Miguel ; Ragauskas, Arthur J. ; Kim, Seong ; Evans, Barbara R. ; Davison, Brian H. ; O'Neill, Hugh. / Hemicellulose-Cellulose Composites Reveal Differences in Cellulose Organization after Dilute Acid Pretreatment. In: Biomacromolecules. 2019 ; Vol. 20, No. 2. pp. 893-903.
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Shah, R, Huang, S, Pingali, SV, Sawada, D, Pu, Y, Rodriguez, M, Ragauskas, AJ, Kim, S, Evans, BR, Davison, BH & O'Neill, H 2019, 'Hemicellulose-Cellulose Composites Reveal Differences in Cellulose Organization after Dilute Acid Pretreatment', Biomacromolecules, vol. 20, no. 2, pp. 893-903. https://doi.org/10.1021/acs.biomac.8b01511

Hemicellulose-Cellulose Composites Reveal Differences in Cellulose Organization after Dilute Acid Pretreatment. / Shah, Riddhi; Huang, Shixin; Pingali, Sai Venkatesh; Sawada, Daisuke; Pu, Yunqiao; Rodriguez, Miguel; Ragauskas, Arthur J.; Kim, Seong; Evans, Barbara R.; Davison, Brian H.; O'Neill, Hugh.

In: Biomacromolecules, Vol. 20, No. 2, 11.02.2019, p. 893-903.

Research output: Contribution to journalArticle

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AU - Shah, Riddhi

AU - Huang, Shixin

AU - Pingali, Sai Venkatesh

AU - Sawada, Daisuke

AU - Pu, Yunqiao

AU - Rodriguez, Miguel

AU - Ragauskas, Arthur J.

AU - Kim, Seong

AU - Evans, Barbara R.

AU - Davison, Brian H.

AU - O'Neill, Hugh

PY - 2019/2/11

Y1 - 2019/2/11

N2 - 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 I β content was increased. Our results point to a tight interaction of xyloglucan with microfibrils while glucomannan only interacts with macrofibril surfaces. This study provides insight into roles of different hemicellulose-cellulose interactions and may help in improving pretreatment processes or engineering plants with decreased recalcitrance.

AB - 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 I β content was increased. Our results point to a tight interaction of xyloglucan with microfibrils while glucomannan only interacts with macrofibril surfaces. This study provides insight into roles of different hemicellulose-cellulose interactions and may help in improving pretreatment processes or engineering plants with decreased recalcitrance.

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