Dependence of Sum Frequency Generation (SFG) Spectral Features on the Mesoscale Arrangement of SFG-Active Crystalline Domains Interspersed in SFG-Inactive Matrix: A Case Study with Cellulose in Uniaxially Aligned Control Samples and Alkali-Treated Secondary Cell Walls of Plants

Makarem, Mohamadamin; Sawada, Daisuke; O'Neill, Hugh M.; Lee, Christopher M.; Kafle, Kabindra; Park, Yong Bum; Mittal, Ashutosh; Kim, Seong H.

doi:10.1021/acs.jpcc.7b02770

Dependence of Sum Frequency Generation (SFG) Spectral Features on the Mesoscale Arrangement of SFG-Active Crystalline Domains Interspersed in SFG-Inactive Matrix: A Case Study with Cellulose in Uniaxially Aligned Control Samples and Alkali-Treated Secondary Cell Walls of Plants

Journal Article · Fri Apr 21 00:00:00 EDT 2017 · Journal of Physical Chemistry. C

DOI:https://doi.org/10.1021/acs.jpcc.7b02770· OSTI ID:1364049

Makarem, Mohamadamin ^[1]; Sawada, Daisuke ^[2]; O'Neill, Hugh M. ^[2]; Lee, Christopher M. ^[1]; Kafle, Kabindra ^[1]; Park, Yong Bum ^[1]; Mittal, Ashutosh ^[3]; Kim, Seong H. ^[1]

Pennsylvania State Univ., University Park, PA (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
National Renewable Energy Lab. (NREL), Golden, CO (United States)

Vibrational sum frequency generation (SFG) spectroscopy can selectively detect not only molecules at two-dimensional (2D) interfaces but also noncentrosymmetric domains interspersed in amorphous three-dimensional (3D) matrixes. However, the SFG analysis of 3D systems is more complicated than 2D systems because more variables are involved. One such variable is the distance between SFG-active domains in SFG-inactive matrixes. In this study, we fabricated control samples in which SFG-active cellulose crystals were uniaxially aligned in an amorphous matrix. Assuming uniform separation distances between cellulose crystals, the relative intensities of alkyl (CH) and hydroxyl (OH) SFG peaks of cellulose could be related to the intercrystallite distance. The experimentally measured CH/OH intensity ratio as a function of the intercrystallite distance could be explained reasonably well with a model constructed using the theoretically calculated hyperpolarizabilities of cellulose and the symmetry cancellation principle of dipoles antiparallel to each other. In conclusion, this comparison revealed physical insights into the intercrystallite distance dependence of the CH/OH SFG intensity ratio of cellulose, which can be used to interpret the SFG spectral features of plant cell walls in terms of mesoscale packing of cellulose microfibrils.

View Accepted Manuscript (DOE)

Research Organization:: National Renewable Energy Laboratory (NREL), Golden, CO (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Biological and Environmental Research (BER) (SC-23); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: AC36-08GO28308; SC0001090

OSTI ID:: 1364049

Report Number(s):: NREL/JA-2700-68692; MainId:18606; UUID:881041c9-8c50-e711-9c0f-2c44fd93e385; MainAdminID:7084

Journal Information:: Journal of Physical Chemistry. C, Journal Name: Journal of Physical Chemistry. C Journal Issue: 18 Vol. 121; ISSN 1932-7447

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

References (51)

On the mechanism of the mercerization of cellulose in wood Revol, J. -F.; Goring, D. A. I. Journal of Applied Polymer Science, Vol. 26, Issue 4 https://doi.org/10.1002/app.1981.070260419	journal	April 1981
Organosolv pretreatment of lignocellulosic biomass for enzymatic hydrolysis Zhao, Xuebing; Cheng, Keke; Liu, Dehua Applied Microbiology and Biotechnology, Vol. 82, Issue 5 https://doi.org/10.1007/s00253-009-1883-1	journal	February 2009
Structure of cellulose and microcrystalline cellulose from various wood species, cotton and flax studied by X-ray scattering Leppänen, Kirsi; Andersson, Seppo; Torkkeli, Mika Cellulose, Vol. 16, Issue 6 https://doi.org/10.1007/s10570-009-9298-9	journal	December 2009
Cellulose microfibril orientation in onion (Allium cepa L.) epidermis studied by atomic force microscopy (AFM) and vibrational sum frequency generation (SFG) spectroscopy Kafle, Kabindra; Xi, Xiaoning; Lee, Christopher M. Cellulose, Vol. 21, Issue 2 https://doi.org/10.1007/s10570-013-0121-2	journal	December 2013
Cellulose polymorphism study with sum-frequency-generation (SFG) vibration spectroscopy: identification of exocyclic CH2OH conformation and chain orientation Lee, Christopher M.; Mittal, Ashutosh; Barnette, Anna L. Cellulose, Vol. 20, Issue 3 https://doi.org/10.1007/s10570-013-9917-3	journal	April 2013
Visualization of the nanoscale pattern of recently-deposited cellulose microfibrils and matrix materials in never-dried primary walls of the onion epidermis Zhang, Tian; Mahgsoudy-Louyeh, Sahar; Tittmann, Bernhard Cellulose, Vol. 21, Issue 2 https://doi.org/10.1007/s10570-013-9996-1	journal	July 2013
Vibrational sum-frequency-generation (SFG) spectroscopy study of the structural assembly of cellulose microfibrils in reaction woods Kafle, Kabindra; Shi, Rui; Lee, Christopher M. Cellulose, Vol. 21, Issue 4 https://doi.org/10.1007/s10570-014-0322-3	journal	June 2014
Comprehensive analysis of cellulose content, crystallinity, and lateral packing in Gossypium hirsutum and Gossypium barbadense cotton fibers using sum frequency generation, infrared and Raman spectroscopy, and X-ray diffraction Lee, Christopher M.; Kafle, Kabindra; Belias, David W. Cellulose, Vol. 22, Issue 2 https://doi.org/10.1007/s10570-014-0535-5	journal	January 2015
Probing crystallinity of never-dried wood cellulose with Raman spectroscopy Agarwal, Umesh P.; Ralph, Sally A.; Reiner, Richard S. Cellulose, Vol. 23, Issue 1 https://doi.org/10.1007/s10570-015-0788-7	journal	October 2015
Comparative physical and chemical analyses of cotton fibers from two near isogenic upland lines differing in fiber wall thickness Kim, Hee Jin; Lee, Christopher M.; Dazen, Kevin Cellulose, Vol. 24, Issue 6 https://doi.org/10.1007/s10570-017-1282-1	journal	April 2017
Effects of Delignification on Crystalline Cellulose in Lignocellulose Biomass Characterized by Vibrational Sum Frequency Generation Spectroscopy and X-ray Diffraction Kafle, Kabindra; Lee, Christopher M.; Shin, Heenae BioEnergy Research, Vol. 8, Issue 4 https://doi.org/10.1007/s12155-015-9627-9	journal	May 2015
Biomass pretreatment: Fundamentals toward application Agbor, Valery B.; Cicek, Nazim; Sparling, Richard Biotechnology Advances, Vol. 29, Issue 6 https://doi.org/10.1016/j.biotechadv.2011.05.005	journal	November 2011
Quantification of crystalline cellulose in lignocellulosic biomass using sum frequency generation (SFG) vibration spectroscopy and comparison with other analytical methods Barnette, Anna L.; Lee, Christopher; Bradley, Laura C. Carbohydrate Polymers, Vol. 89, Issue 3 https://doi.org/10.1016/j.carbpol.2012.04.014	journal	July 2012
Characterization of cellulose I/II hybrid fibers isolated from energycane bagasse during the delignification process: Morphology, crystallinity and percentage estimation Yue, Yiying; Han, Jingquan; Han, Guangping Carbohydrate Polymers, Vol. 133 https://doi.org/10.1016/j.carbpol.2015.07.058	journal	November 2015
Super-resolution Microscopy in Plant Cell Imaging Komis, George; Šamajová, Olga; Ovečka, Miroslav Trends in Plant Science, Vol. 20, Issue 12 https://doi.org/10.1016/j.tplants.2015.08.013	journal	December 2015
Hydrogen-Bonding Network and OH Stretch Vibration of Cellulose: Comparison of Computational Modeling with Polarized IR and SFG Spectra Lee, Christopher M.; Kubicki, James D.; Fan, Bingxin The Journal of Physical Chemistry B, Vol. 119, Issue 49 https://doi.org/10.1021/acs.jpcb.5b08015	journal	November 2015
Multimodal Broadband Vibrational Sum Frequency Generation (MM-BB-V-SFG) Spectrometer and Microscope Lee, Christopher M.; Kafle, Kabindra; Huang, Shixin The Journal of Physical Chemistry B, Vol. 120, Issue 1 https://doi.org/10.1021/acs.jpcb.5b10290	journal	December 2015
Quantum Mechanical Calculations of Vibrational Sum-Frequency-Generation (SFG) Spectra of Cellulose: Dependence of the CH and OH Peak Intensity on the Polarity of Cellulose Chains within the SFG Coherence Domain Lee, Christopher M.; Chen, Xing; Weiss, Philip A. The Journal of Physical Chemistry Letters, Vol. 8, Issue 1 https://doi.org/10.1021/acs.jpclett.6b02624	journal	December 2016
Selective Detection of Crystalline Cellulose in Plant Cell Walls with Sum-Frequency-Generation (SFG) Vibration Spectroscopy Barnette, Anna L.; Bradley, Laura C.; Veres, Brandon D. Biomacromolecules, Vol. 12, Issue 7 https://doi.org/10.1021/bm200518n	journal	July 2011
Crystal Structure and Hydrogen-Bonding System in Cellulose Iβ from Synchrotron X-ray and Neutron Fiber Diffraction Nishiyama, Yoshiharu; Langan, Paul; Chanzy, Henri Journal of the American Chemical Society, Vol. 124, Issue 31 https://doi.org/10.1021/ja0257319	journal	August 2002
Crystal Structure and Hydrogen Bonding System in Cellulose I _α from Synchrotron X-ray and Neutron Fiber Diffraction Nishiyama, Yoshiharu; Sugiyama, Junji; Chanzy, Henri Journal of the American Chemical Society, Vol. 125, Issue 47 https://doi.org/10.1021/ja037055w	journal	November 2003
Sum-Frequency-Generation Vibration Spectroscopy and Density Functional Theory Calculations with Dispersion Corrections (DFT-D2) for Cellulose Iα and Iβ Lee, Christopher M.; Mohamed, Naseer M. A.; Watts, Heath D. The Journal of Physical Chemistry B, Vol. 117, Issue 22 https://doi.org/10.1021/jp402998s	journal	May 2013
Mercerization of primary wall cellulose and its implication for the conversion of cellulose I→cellulose II Dinand, Elizabeth; Vignon, Michel; Chanzy, Henri Cellulose, Vol. 9, Issue 1, p. 7-18 https://doi.org/10.1023/A:1015877021688	journal	March 2002
Random quasi-phase-matching in bulk polycrystalline isotropic nonlinear materials Baudrier-Raybaut, M.; Haïdar, R.; Kupecek, Ph. Nature, Vol. 432, Issue 7015 https://doi.org/10.1038/nature03027	journal	November 2004
Folding of xylan onto cellulose fibrils in plant cell walls revealed by solid-state NMR Simmons, Thomas J.; Mortimer, Jenny C.; Bernardinelli, Oigres D. Nature Communications, Vol. 7, Issue 1 https://doi.org/10.1038/ncomms13902	journal	December 2016
Growth of the plant cell wall Cosgrove, Daniel J. Nature Reviews Molecular Cell Biology, Vol. 6, Issue 11, p. 850-861 https://doi.org/10.1038/nrm1746	journal	November 2005
Progressive structural changes of Avicel, bleached softwood and bacterial cellulose during enzymatic hydrolysis Kafle, Kabindra; Shin, Heenae; Lee, Christopher M. Scientific Reports, Vol. 5, Issue 1 https://doi.org/10.1038/srep15102	journal	October 2015
Cellulose nanomaterials review: structure, properties and nanocomposites Moon, Robert J.; Martini, Ashlie; Nairn, John Chemical Society Reviews, Vol. 40, Issue 7 https://doi.org/10.1039/c0cs00108b	journal	January 2011
Multi-scale visualization and characterization of lignocellulosic plant cell wall deconstruction during thermochemical pretreatment Chundawat, Shishir P. S.; Donohoe, Bryon S.; da Costa Sousa, Leonardo Energy & Environmental Science, Vol. 4, Issue 3, 973 https://doi.org/10.1039/c0ee00574f	journal	January 2011
Probing crystal structure and mesoscale assembly of cellulose microfibrils in plant cell walls, tunicate tests, and bacterial films using vibrational Sum Frequency Generation (SFG) spectroscopy Lee, Christopher M.; Kafle, Kabindra; Park, Yong Bum Physical Chemistry Chemical Physics, Vol. 16, Issue 22 https://doi.org/10.1039/c4cp00515e	journal	January 2014
Structural models of primary cell walls in flowering plants: consistency of molecular structure with the physical properties of the walls during growth. Carpita, Nc; Gibeaut, Dm The Plant Journal, Vol. 3, Issue 1 https://doi.org/10.1046/j.1365-313X.1993.00999.x	journal	January 1993
Nanostructure of cellulose microfibrils in spruce wood Fernandes, A. N.; Thomas, L. H.; Altaner, C. M. Proceedings of the National Academy of Sciences, Vol. 108, Issue 47 https://doi.org/10.1073/pnas.1108942108	journal	November 2011
Quantitative spectral and orientational analysis in surface sum frequency generation vibrational spectroscopy (SFG-VS) Wang *, Hong-Fei; Gan † ‡, Wei; Lu † ‡ §, Rong International Reviews in Physical Chemistry, Vol. 24, Issue 2 https://doi.org/10.1080/01442350500225894	journal	April 2005
Implementing the Theory of Sum Frequency Generation Vibrational Spectroscopy: A Tutorial Review Lambert, Alex G.; Davies, Paul B.; Neivandt, David J. Applied Spectroscopy Reviews, Vol. 40, Issue 2 https://doi.org/10.1081/ASR-200038326	journal	May 2005
A Revised Architecture of Primary Cell Walls Based on Biomechanical Changes Induced by Substrate-Specific Endoglucanases Park, Yong Bum; Cosgrove, Daniel J. Plant Physiology, Vol. 158, Issue 4 https://doi.org/10.1104/pp.111.192880	journal	February 2012
Structure of Cellulose Microfibrils in Primary Cell Walls from Collenchyma Thomas, Lynne H.; Forsyth, V. Trevor; Šturcová, Adriana Plant Physiology, Vol. 161, Issue 1 https://doi.org/10.1104/pp.112.206359	journal	November 2012
Monitoring Meso-Scale Ordering of Cellulose in Intact Plant Cell Walls Using Sum Frequency Generation Spectroscopy Park, Y. B.; Lee, C. M.; Koo, B. -W. PLANT PHYSIOLOGY, Vol. 163, Issue 2 https://doi.org/10.1104/pp.113.225235	journal	August 2013
Wall Structure and Wall Loosening. A Look Backwards and Forwards: Fig. 1. Cosgrove, Daniel J. Plant Physiology, Vol. 125, Issue 1 https://doi.org/10.1104/pp.125.1.131	journal	January 2001
Cell wall extension results in the coordinate separation of parallel microfibrils: evidence from scanning electron microscopy and atomic force microscopy: Creep and cell wall ultrastructure Marga, Francoise; Grandbois, Michel; Cosgrove, Daniel J. The Plant Journal, Vol. 43, Issue 2 https://doi.org/10.1111/j.1365-313X.2005.02447.x	journal	June 2005
Spatial organization of cellulose microfibrils and matrix polysaccharides in primary plant cell walls as imaged by multichannel atomic force microscopy Zhang, Tian; Zheng, Yunzhen; Cosgrove, Daniel J. The Plant Journal, Vol. 85, Issue 2 https://doi.org/10.1111/tpj.13102	journal	January 2016
Toward a Systems Approach to Understanding Plant Cell Walls Somerville, C. Science, Vol. 306, Issue 5705 https://doi.org/10.1126/science.1102765	journal	December 2004
Biomass Recalcitrance: Engineering Plants and Enzymes for Biofuels Production Himmel, M. E.; Ding, S.-Y.; Johnson, D. K. Science, Vol. 315, Issue 5813, p. 804-807 https://doi.org/10.1126/science.1137016	journal	February 2007
How Does Plant Cell Wall Nanoscale Architecture Correlate with Enzymatic Digestibility? Ding, S. -Y.; Liu, Y. -S.; Zeng, Y. Science, Vol. 338, Issue 6110 https://doi.org/10.1126/science.1227491	journal	November 2012
Cellulose Synthesis in Higher Plants Somerville, Chris Annual Review of Cell and Developmental Biology, Vol. 22, Issue 1 https://doi.org/10.1146/annurev.cellbio.22.022206.160206	journal	November 2006
Perturbation of Brachypodium distachyon CELLULOSE SYNTHASE A4 or 7 results in abnormal cell walls Handakumbura, Pubudu P.; Matos, Dominick A.; Osmont, Karen S. BMC Plant Biology, Vol. 13, Issue 1 https://doi.org/10.1186/1471-2229-13-131	journal	January 2013
Cell wall structural changes in wheat straw pretreated for bioethanol production Kristensen, Jan B.; Thygesen, Lisbeth G.; Felby, Claus Biotechnology for Biofuels, Vol. 1, Issue 1 https://doi.org/10.1186/1754-6834-1-5	journal	January 2008
Effects of alkaline or liquid-ammonia treatment on crystalline cellulose: changes in crystalline structure and effects on enzymatic digestibility Mittal, Ashutosh; Katahira, Rui; Himmel, Michael E. Biotechnology for Biofuels, Vol. 4, Issue 1 https://doi.org/10.1186/1754-6834-4-41	journal	January 2011
Effect of mechanical disruption on the effectiveness of three reactors used for dilute acid pretreatment of corn stover Part 1: chemical and physical substrate analysis Wang, Wei; Chen, Xiaowen; Donohoe, Bryon S. Biotechnology for Biofuels, Vol. 7, Issue 1 https://doi.org/10.1186/1754-6834-7-57	journal	January 2014
Plant Cell Walls Albersheim, Peter; Darvill, Alan; Roberts, Keith Garland Science https://doi.org/10.1201/9780203833476	book	April 2010
Sum Frequency Generation Microscopy Study of Cellulose Fibers Hieu, Hoang Chi; Tuan, Nguyen Anh; Li, Hongyan Applied Spectroscopy, Vol. 65, Issue 11 https://doi.org/10.1366/11-06388	journal	November 2011
Structure of an Acidic Xylan Isolated from Birch Wood Holocellulose. Saarnio, Jouko; Wathen, Kristina; Gustafsson, Charley Acta Chemica Scandinavica, Vol. 8 https://doi.org/10.3891/acta.chem.scand.08-0825	journal	January 1954

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