Structural Insights into Low and High Recalcitrance Natural Poplar Variants Using Neutron and X-ray Scattering

Riddhi Shah; Samarthya Bhagia; Jong K. Keum; Sai Venkatesh Pingali; Arthur J. Ragauskas; Brian H. Davison; Hugh O'Neill

doi:10.1021/acssuschemeng.0c05251

Structural Insights into Low and High Recalcitrance Natural Poplar Variants Using Neutron and X-ray Scattering

Riddhi Shah, Samarthya Bhagia, Jong K. Keum, Sai Venkatesh Pingali, Arthur J. Ragauskas, Brian H. Davison, Hugh O'Neill

Research output: Contribution to journal › Article › peer-review

9 Scopus citations

Abstract

We used small-angle neutron scattering (SANS) and wide-angle X-ray scattering (WAXS) to study two Populus trichocarpa variants, GW-11012 and BESC-316, with lignin contents of 17.8 and 23.2%, respectively, to understand why the low lignin variant has increased sugar release during liquid hot water (LHW) pretreatment. SANS showed differences in cell wall polymer arrangement in the variants. In GW-11012, the cellulose microfibrils were similar in size to BESC-316 but were not equally spaced and lignin was aggregated rather than homogenously interspersed with other matrix co-polymers. However, after LHW pretreatments, the SANS profiles of the pretreated variants were almost indistinguishable, indicating that the nanoscale structural features could not adequately explain the increased sugar release observed in GW-11012. WAXS analysis revealed higher cellulose crystallinity and larger crystallite size in native and pretreated GW-11012. However, the most significant difference was that the crystallite orientation was approximately 2-fold higher in GW-11012. This suggests that higher crystallite orientation may be favorable for the action of processive cellulases leading to increased sugar release from GW-11012. Our study shows that there is a complex interplay between cell wall polymers during their deposition resulting in changes in lignin distribution and cellulose structure, highlighting the importance of investigating plant cell wall architecture across multiple length scales.

Original language	English
Pages (from-to)	13838-13849
Number of pages	12
Journal	ACS Sustainable Chemistry and Engineering
Volume	8
Issue number	36
DOIs	https://doi.org/10.1021/acssuschemeng.0c05251
State	Published - Sep 14 2020

Funding

R.S., S.B., S.V.P., A.J.R., H.O., and B.H.D. acknowledge the support of the Genomic Science Program, Office of Biological and Environmental Research (OBER), U. S. Department of Energy (DOE), under contract FWP ERKP752 for this research. The natural poplar variants used in this study were provided by the Center for Bioenergy Innovation (CBI). Thermochemical pretreatment and WAXS measurements were performed at the Center for Nanophase Materials Sciences (CNMS) supported by the Office of Basic Energy Sciences (BES), DOE. The SANS studies on Bio-SANS were supported by the OBER funded Center for Structural Molecular Biology (CSMB) under contract FWP ERKP291, using the High Flux Isotope Reactor supported by the BES, DOE. This manuscript has been authored by UT-Battelle, LLC under contract no. DE-AC05-00OR22725 with the U.S. Department of Energy. The United States Government retains and the publisher, by accepting the article for publication, acknowledges that the United States government retains a nonexclusive, paid-up, irrevocable, world-wide license to publish or reproduce the published form of this manuscript, or allow others to do so, for United States government purposes. The Department of Energy will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan ( http://energy.gov/downloads/doe-public-access-plan )

Keywords

cell wall structure
cellulose
lignin
liquid hot water pretreatment
poplar
small-angle neutron scattering
wide-angle X-ray scattering

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10.1021/acssuschemeng.0c05251

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title = "Structural Insights into Low and High Recalcitrance Natural Poplar Variants Using Neutron and X-ray Scattering",

abstract = "We used small-angle neutron scattering (SANS) and wide-angle X-ray scattering (WAXS) to study two Populus trichocarpa variants, GW-11012 and BESC-316, with lignin contents of 17.8 and 23.2%, respectively, to understand why the low lignin variant has increased sugar release during liquid hot water (LHW) pretreatment. SANS showed differences in cell wall polymer arrangement in the variants. In GW-11012, the cellulose microfibrils were similar in size to BESC-316 but were not equally spaced and lignin was aggregated rather than homogenously interspersed with other matrix co-polymers. However, after LHW pretreatments, the SANS profiles of the pretreated variants were almost indistinguishable, indicating that the nanoscale structural features could not adequately explain the increased sugar release observed in GW-11012. WAXS analysis revealed higher cellulose crystallinity and larger crystallite size in native and pretreated GW-11012. However, the most significant difference was that the crystallite orientation was approximately 2-fold higher in GW-11012. This suggests that higher crystallite orientation may be favorable for the action of processive cellulases leading to increased sugar release from GW-11012. Our study shows that there is a complex interplay between cell wall polymers during their deposition resulting in changes in lignin distribution and cellulose structure, highlighting the importance of investigating plant cell wall architecture across multiple length scales.",

keywords = "cell wall structure, cellulose, lignin, liquid hot water pretreatment, poplar, small-angle neutron scattering, wide-angle X-ray scattering",

author = "Riddhi Shah and Samarthya Bhagia and Keum, {Jong K.} and Pingali, {Sai Venkatesh} and Ragauskas, {Arthur J.} and Davison, {Brian H.} and Hugh O'Neill",

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AU - Shah, Riddhi

AU - Bhagia, Samarthya

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AU - Pingali, Sai Venkatesh

AU - Ragauskas, Arthur J.

AU - Davison, Brian H.

AU - O'Neill, Hugh

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N2 - We used small-angle neutron scattering (SANS) and wide-angle X-ray scattering (WAXS) to study two Populus trichocarpa variants, GW-11012 and BESC-316, with lignin contents of 17.8 and 23.2%, respectively, to understand why the low lignin variant has increased sugar release during liquid hot water (LHW) pretreatment. SANS showed differences in cell wall polymer arrangement in the variants. In GW-11012, the cellulose microfibrils were similar in size to BESC-316 but were not equally spaced and lignin was aggregated rather than homogenously interspersed with other matrix co-polymers. However, after LHW pretreatments, the SANS profiles of the pretreated variants were almost indistinguishable, indicating that the nanoscale structural features could not adequately explain the increased sugar release observed in GW-11012. WAXS analysis revealed higher cellulose crystallinity and larger crystallite size in native and pretreated GW-11012. However, the most significant difference was that the crystallite orientation was approximately 2-fold higher in GW-11012. This suggests that higher crystallite orientation may be favorable for the action of processive cellulases leading to increased sugar release from GW-11012. Our study shows that there is a complex interplay between cell wall polymers during their deposition resulting in changes in lignin distribution and cellulose structure, highlighting the importance of investigating plant cell wall architecture across multiple length scales.

AB - We used small-angle neutron scattering (SANS) and wide-angle X-ray scattering (WAXS) to study two Populus trichocarpa variants, GW-11012 and BESC-316, with lignin contents of 17.8 and 23.2%, respectively, to understand why the low lignin variant has increased sugar release during liquid hot water (LHW) pretreatment. SANS showed differences in cell wall polymer arrangement in the variants. In GW-11012, the cellulose microfibrils were similar in size to BESC-316 but were not equally spaced and lignin was aggregated rather than homogenously interspersed with other matrix co-polymers. However, after LHW pretreatments, the SANS profiles of the pretreated variants were almost indistinguishable, indicating that the nanoscale structural features could not adequately explain the increased sugar release observed in GW-11012. WAXS analysis revealed higher cellulose crystallinity and larger crystallite size in native and pretreated GW-11012. However, the most significant difference was that the crystallite orientation was approximately 2-fold higher in GW-11012. This suggests that higher crystallite orientation may be favorable for the action of processive cellulases leading to increased sugar release from GW-11012. Our study shows that there is a complex interplay between cell wall polymers during their deposition resulting in changes in lignin distribution and cellulose structure, highlighting the importance of investigating plant cell wall architecture across multiple length scales.

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KW - liquid hot water pretreatment

KW - poplar

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ER -

Structural Insights into Low and High Recalcitrance Natural Poplar Variants Using Neutron and X-ray Scattering

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