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Hydrogen bonding and other non-covalent interactions at the surfaces of cellulose microfibrils

CELLULOSE (2023)

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Article Biochemistry & Molecular Biology

Potent Time-Dependent Ice Recrystallization Inhibition Activity of Cellulose Nanocrystals in Sucrose Solutions

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Summary: This study found that cellulose nanocrystals (CNCs) exhibit ice recrystallization inhibition (IRI) activity over longer exposure times in a model ice cream system. The time-dependent surface coverage of CNCs on ice crystals appears to be a key mechanism for inhibiting ice crystal growth. These findings emphasize the importance of selecting a suitable exposure time to evaluate IRI activity of new materials involving CNCs.

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Cellulose and the role of hydrogen bonds: not in charge of everything

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Summary: In the cellulose scientific community, hydrogen bonding is often exaggerated in its importance, as it is just one of several molecular interactions and relatively weak, sensitive to the environment.

CELLULOSE (2022)

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Review Materials Science, Paper & Wood

On the organization of hemicelluloses in the wood cell wall

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Summary: The structural arrangement of polymers in the cell wall of wood, particularly the roles of glucomannan and xylan in the secondary cell wall, is still not fully understood. Recent studies have shown a close association of xylan with cellulose microfibrils in softwoods. Various techniques have been used to examine these findings, and the overall results strongly support the association of both glucomannan and xylan with cellulose microfibrils.

CELLULOSE (2022)

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Review Physics, Condensed Matter

Understanding Hydrophobic Effects: Insights from Water Density Fluctuations

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Summary: The study of hydrophobic effects is crucial in materials science, biology, and related fields. This review explores the theoretical, computational, and experimental developments that have contributed to our understanding of this phenomenon. It discusses the role of density fluctuations in bulk water in explaining the differences in hydration between molecular and macroscopic solutes, as well as the influence of chemical and topographical patterns on surface hydrophobicity. The review also highlights the use of interfacial water density fluctuations to characterize complex surfaces, such as proteins, and their mediating interactions. Overall, this review provides insights into the thermodynamic forces and desolvation barriers that drive hydrophobic interactions.

ANNUAL REVIEW OF CONDENSED MATTER PHYSICS (2022)

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Article Multidisciplinary Sciences

Carbohydrate-aromatic interface and molecular architecture of lignocellulose

Alex Kirui et al.

Summary: In this study, the assembly of lignocellulosic components in plant stems and the interactions between polysaccharides and the aromatic polymer lignin are investigated using solid-state NMR spectroscopy. The research shows that the extent of glycan-aromatic association varies in different types of plant stems, and lignin primarily interacts with xylan through non-covalent interactions and partially binds to the junction of xylan and cellulose surface. The unique feature of homogeneous mixing of all molecules in softwoods enables better water retention. These findings provide insights into the principles of polymer interactions underlying the heterogeneous architecture of lignocellulose, which can guide the rational design of more digestible plants and more efficient biomass-conversion pathways.

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Quantifying the Contribution of the Dispersion Interaction and Hydrogen Bonding to the Anisotropic Elastic Properties of Chitin and Chitosan

Pan Chen et al.

Summary: This study calculated the elastic tensors of chitin and chitosan allomorphs using density functional theory and compared them with experimental values. The results showed that the modulus varied in different directions and switching off the dispersion correction led to a decrease in modulus.

BIOMACROMOLECULES (2022)

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Article Biochemical Research Methods

A 13C three-dimensional DQ-SQ-SQ correlation experiment for high-resolution analysis of complex carbohydrates using solid-state NMR

S. Chandra Shekar et al.

Summary: The study presents a new method for analyzing the structure of carbohydrates using solid-state NMR. The method provides high resolution and allows for accurate resonance assignment of polysaccharides in plant and fungal cell walls using uniformly labeled cells. Long-range structural restraints can be obtained, which contributes to a better understanding of the spatial organization of plant cellulose microfibrils. The method has broad applications in the study of cellular carbohydrates and carbon-based biomaterials.

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Review Plant Sciences

Building an extensible cell wall

Daniel J. Cosgrove

Summary: This article discusses the evolution of primary cell wall structure and the mechanism of surface enlargement, highlighting the role of cellulose, xyloglucan, and pectins. By using molecular dynamics methods, a quantitative model is developed to understand the mechanical behavior of the cell wall, revealing the dominant role of cellulose-cellulose interactions in forming a strong yet extensible network.

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Do antifreeze proteins generally possess the potential to promote ice growth?

Shaoli Cui et al.

Summary: This study investigates the effect of different antifreeze proteins (AFPs) on the growth of ice crystals on the basal and prismatic surfaces. The results show that only hyperactive AFPs can promote the growth of the basal plane, while moderately active AFPs cannot. Furthermore, no significant promotion is observed on the prismatic plane. This promotion may be attributed to the thicker ice/water interface on the basal plane and the synergy between hypAFPs and ice crystals.

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Article Biotechnology & Applied Microbiology

Solid-state NMR of unlabeled plant cell walls: high-resolution structural analysis without isotopic enrichment

Wancheng Zhao et al.

Summary: The study presented a method using Dynamic Nuclear Polarization (DNP) to enhance sensitivity and eliminate the need for isotopic labeling, successfully collecting 2D C-13-C-13 correlation spectra. The atomic resolution revealed the polymorphic structure of cellulose and xylan, while NMR relaxation and dipolar order parameters indicated changes in molecular motions in a double mutant. By skipping isotopic labeling, the DNP strategy is universally applicable to all lignocellulose materials, providing a time-efficient method for understanding polysaccharide structure and cell wall assembly in various plant tissues and species.

BIOTECHNOLOGY FOR BIOFUELS (2021)

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Review Chemistry, Applied

Combining scattering analysis and atomistic simulation of wood-water interactions

Paavo A. Penttila et al.

Summary: This article explores the molecular-scale interactions between water and cellulose microfibril bundles in plant cell walls, discussing new methods using X-ray and neutron scattering analysis and atomistic simulations, envisioning future research directions, and discussing opportunities in the application of lignocellulosic materials.

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Article Chemistry, Applied

Hydrogen bonds dominated frictional stick-slip of cellulose nanocrystals

Chi Zhang et al.

Summary: Through atomistic simulation, the mechanical behavior of cellulose-cellulose nanocrystal hydrophilic interface was studied, showing the central role of interfacial hydrogen bonds in explaining various findings. The friction force generated by a single hydrogen bond was estimated to be around 1.3 E-10 N under a shearing speed of 1 m/s.

CARBOHYDRATE POLYMERS (2021)

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Article Biochemistry & Molecular Biology

Importance of Water in Maintaining Softwood Secondary Cell Wall Nanostructure

Rosalie Cresswell et al.

Summary: Water plays a critical role at the hemicellulose-cellulose interface in the molecular architecture of softwood secondary cell walls. After dehydration, molecular shrinkage occurs and the original conformation is not fully recovered upon rehydration. These irreversible nanostructural changes provide a basis for understanding and enhancing the properties of wood-based materials.

BIOMACROMOLECULES (2021)

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Water-accessibility of interfibrillar spaces in spruce wood cell walls

Paavo A. Penttila et al.

Summary: The water-accessibility of nanoscale pores within unmodified Norway spruce cell walls was studied using SANS and FTIR, revealing two distinct processes of water exchange between cellulose microfibrils with different timescales - one occurring within minutes and the other continuing for weeks.

CELLULOSE (2021)

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Deswelling of microfibril bundles in drying wood studied by small-angle neutron scattering and molecular dynamics

Aleksi Zitting et al.

Summary: The structural changes of cellulose microfibrils and microfibril bundles in unmodified spruce cell wall due to drying in air were investigated using time-resolved small-angle neutron scattering. The experiments and simulations revealed that individual cellulose microfibrils remain relatively unaffected by drying, while there is a significant decrease in fibril-to-fibril distances in microfibril bundles. Two distinct drying regions, constant-rate drying and falling-rate drying, were observed during the experiments, supported by molecular dynamics simulations.

CELLULOSE (2021)

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Quantifying the influence of dispersion interactions on the elastic properties of crystalline cellulose

Pan Chen et al.

Summary: Dispersion and electrostatic interactions play significant roles in the assembly of macromolecular chains in crystalline polysaccharides. Using dispersion-corrected DFT calculations, the exact contribution of dispersion to stiffness at the molecular level in different crystalline cellulose structures was quantified.

CELLULOSE (2021)

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Common sorption isotherm models are not physically valid for water in wood

Emil E. Thybring et al.

Summary: Sorption isotherm models are commonly used to understand water interactions with cellulosic materials, but they do not accurately predict physical properties in wood.

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Affinity of small-molecule solutes to hydrophobic, hydrophilic, and chemically patterned interfaces in aqueous solution

Jacob Monroe et al.

Summary: The performance of membranes in water purification, especially in terms of fouling resistance, is influenced by the interactions between solvated species and membrane surfaces. Efforts to create fouling-resistant membranes often focus on hydrophilization of surfaces. However, molecular simulations show that solutes are attracted to both hydrophobic and hydrophilic surfaces, contradicting macroscopic measures which suggest solute affinity is higher on hydrophobic surfaces. This suggests that traditional macroscopic hydrophobicity metrics may not accurately predict solute-surface affinity, and that molecular-scale surface chemical patterning plays a significant role in influencing affinity.

PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA (2021)

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Nanostructural deformation of high-stiffness spruce wood under tension

Lynne H. Thomas et al.

Summary: Research has shown that the cellulose microfibrils in conifer wood stretch together under tension, with stress relaxation facilitated by water. The role of hemicelluloses in affecting the stretching and relaxation behavior of cellulose microfibrils was also observed. Additionally, it was found that lignin and hemicellulosic glucomannans may contribute to stress transfer between microfibril bundles on a larger scale.

SCIENTIFIC REPORTS (2021)

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Article Biochemical Research Methods

Anisotropy of transverse and longitudinal relaxations in liquids entrapped in nano- and micro-cavities of a plant stem

Gregory Furman et al.

Summary: This study experimented and modeled the anisotropy of H-1 NMR spin-lattice and spin-spin relaxations in fresh celery stem, revealing the presence of water-filled nano- and micro-cavities that are elongated and related to non-spherical vascular cells. Good agreement between experimental data and theoretical results was achieved by adjusting fitting parameters, indicating noticeable ordering of the water-filled cavities in the celery stem. The approach allows experimental determination of order parameters of microscopic vascular structures in plants using NMR technique.

JOURNAL OF MAGNETIC RESONANCE (2021)

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Article Chemistry, Physical

Direct Evidence for Aligned Binding of Cellulase Enzymes to Cellulose Surfaces

Kayla Sprenger et al.

Summary: Engineers have been designing new cellulase enzymes for the conversion of biomass into green fuels and chemicals, with a critical factor being the attachment via the enzyme's carbohydrate binding module (CBM). Experimental data and molecular dynamics simulations show that binding is driven by hydrogen bonding and that tyrosine side chains within the CBM align the cellulase with the registry of the cellulose surface. This alignment is favorable for the translocation and effective cellulose breakdown, likely an important parameter for the design of novel enzymes.

JOURNAL OF PHYSICAL CHEMISTRY LETTERS (2021)

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Article Materials Science, Paper & Wood

Spontaneous rearrangement of acetylated xylan on hydrophilic cellulose surfaces

Madhulika Gupta et al.

Summary: The interaction between xylan and cellulose microfibrils is crucial for secondary cell wall strength, with acetate or glucuronic acid substitutions on xylan shown to influence these interactions. Depending on the position and nature of the substitution, xylans can adopt different helical screw conformations when interacting with the hydrophilic face of cellulose fibers. These findings point to the importance of evenly spaced chemical functionalization in tuning xylan-cellulose interactions and stabilizing specific helical conformations on the cellulose surface.

CELLULOSE (2021)

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Article Materials Science, Paper & Wood

Moisture induced straining of the cellulosic microfibril

Lennart Salmen et al.

Summary: Moisture absorption in wood cell wall structure causes swelling of wood due to sorptive action of carbohydrate wood polymers, leading to transverse contraction and slight elongation of cellulose crystals. These deformations are reversible during moisture desorption, attributed to swelling forces from longitudinal and lateral expansions of non-crystalline cellulose molecules and hemicellulose.

CELLULOSE (2021)

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Article Polymer Science

Process-dependent nanostructures of regenerated cellulose fibres revealed by small angle neutron scattering

Daisuke Sawada et al.

Summary: The nanometric internal structure of polymeric fibres plays a vital role in their mechanical properties. This study examined the correlation between structural parameters and mechanical properties of regenerated cellulose fibres prepared using various spinning technologies, finding a high correlation in the former group but lower correlation in the latter group. These structural parameters serve as a basis for understanding the structure-property relationship and optimizing fibre production based on spinning types and conditions.

POLYMER (2021)

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The atomistic details of the ice recrystallisation inhibition activity of PVA

Fabienne Bachtiger et al.

Summary: Understanding ice recrystallisation is crucial for improving current cryopreservation technologies. The authors combine experiments and simulations to reveal the atomistic details of the ice recrystallization inhibition (IRI) activity of poly(vinyl)alcohol-the most potent biomimetic IRI agent.

NATURE COMMUNICATIONS (2021)

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Entropy drives the adsorption of xyloglucan to cellulose surfaces-A molecular dynamics study

Saina Kishani et al.

Summary: This study investigated the thermodynamics of the adsorption of xyloglucan (XG) to cellulose surfaces at different temperatures using molecular dynamics simulations. The results showed that adsorption near room temperature is an endothermic process driven by the entropy of released interfacial water molecules. In the case of native cellulose, adsorption became exothermic at higher temperatures, while the interactions between water and charged groups of oxidized cellulose hindered this transition.

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How Microscopic Features of Mineral Surfaces Critically Influence Heterogeneous Ice Nucleation

Abhishek Soni et al.

Summary: Heterogeneous ice nucleation, driven by lattice match and surface morphology, is crucial for environmental, biological, and atmospheric science. Molecular simulations were used to study the effects of these factors on atmospherically relevant minerals, revealing the importance of 2D lattice perspectives in understanding and predicting ice nucleation. The research aims to contribute to a general understanding of ice nucleation by various surfaces.

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Cellulose Nanocrystals Facilitate Needle-like Ice Crystal Growth and Modulate Molecular Targeted Ice Crystal Nucleation

Yi Hou et al.

Summary: Ice nucleators play crucial roles in various fields, but their complicated extract and biocompatibility remain unresolved. This study demonstrates that nanocrystalline cellulose materials have special properties to enhance ice nucleation and ice crystal growth, revealing a molecular level mechanism behind it.

NANO LETTERS (2021)

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Unique reactivity of nanoporous cellulosic materials mediated by surface-confined water

Marco Beaumont et al.

Summary: By utilizing surface-bound water in nanoporous cellulosic fibers, this study demonstrates an increase in the reaction rate of surface acetylation reactions and enables regioselectivity of the reaction, outperforming reactions occurring in organic solvents in terms of efficiency and environmental compatibility.

NATURE COMMUNICATIONS (2021)

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Nanoscale Wetting of Crystalline Cellulose

Lucas N. Trentin et al.

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BIOMACROMOLECULES (2021)

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Dynamical Water Ingress and Dissolution at the Amorphous-Crystalline Cellulose Interface

Yuxiang Wang et al.

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BIOMACROMOLECULES (2021)

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Xylan Structure and Dynamics in Native Brachypodium Grass Cell Walls Investigated by Solid-State NMR Spectroscopy

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Summary: The polysaccharide composition and dynamics of intact stem and leaf cell walls in the model grass Brachypodium distachyon were studied, revealing differences in xylan and cellulose content between stem and leaf cell walls at various developmental stages. Additionally, acetylated xylan chains were found to interact more extensively with cellulose in the stem, promoting cellulose lignin interactions essential for secondary cell wall formation.

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Gradients in Wall Mechanics and Polysaccharides along Growing Inflorescence Stems

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Dynamics of water bound to crystalline cellulose

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Different Conformations of Surface Cellulose Molecules in Native Cellulose Microfibrils Revealed by Layer-by-Layer Peeling

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Quantification of a tightly adsorbed monolayer of xylan on cellulose surface

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Metrics of rhamnogalacturonan I with β-(1→4)-galactan side chains and structural basis for its self-aggregation

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Physical properties of cellulosic materials related to moisture changes

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WOOD SCIENCE AND TECHNOLOGY (2016)

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Cellulose Structural Polymorphism in Plant Primary Cell Walls Investigated by High-Field 2D Solid-State NMR Spectroscopy and Density Functional Theory Calculations

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BIOMACROMOLECULES (2016)

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13C NMR assignments of regenerated cellulose from solid-state 2D NMR spectroscopy

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Non-exchanging hydroxyl groups on the surface of cellulose fibrils: The role of interaction with water

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Equilibrium thermodynamics of wood moisture revisited: presentation of a simplified theory

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Chemical, colloidal and mechanical contributions to the state of water in wood cell walls

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NEW JOURNAL OF PHYSICS (2016)

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Spatial organization of cellulose microfibrils and matrix polysaccharides in primary plant cell walls as imaged by multichannel atomic force microscopy

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PLANT JOURNAL (2016)

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Cellulose synthase complexes act in a concerted fashion to synthesize highly aggregated cellulose in secondary cell walls of plants

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PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA (2016)

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SOLID STATE NUCLEAR MAGNETIC RESONANCE (2016)

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Probing the Molecular Architecture of Arabidopsis thaliana Secondary Cell Walls Using Two- and Three-Dimensional 13C Solid State Nuclear Magnetic Resonance Spectroscopy

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Diffraction evidence for the structure of cellulose microfibrils in bamboo, a model for grass and cereal celluloses

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BMC PLANT BIOLOGY (2015)

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Hydrated fractions of cellulosics probed by infrared spectroscopy coupled with dynamics of deuterium exchange

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Prediction of Conformationally Dependent Atomic Multipole Moments in Carbohydrates

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Cellulose-Pectin Spatial Contacts Are Inherent to Never-Dried Arabidopsis Primary Cell Walls: Evidence from Solid-State Nuclear Magnetic Resonance

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Electron (charge) density studies of cellulose models

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Atomic partial charges and one Lennard-Jones parameter crucial to model cellulose allomorphs

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Water-Polysaccharide Interactions in the Primary Cell Wall of Arabidopsis thaliana from Polarization Transfer Solid-State NMR

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Out-of-plane orientation of cellulose elementary fibrils on spruce tracheid wall based on imaging with high-resolution transmission electron microscopy

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Hydrostatic pressure and temperature dependence of wood moisture sorption isotherms

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Sensitivity-enhanced solid-state NMR detection of expansin's target in plant cell walls

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Pectin-Cellulose Interactions in the Arabidopsis Primary Cell Wall from Two-Dimensional Magic-Angle-Spinning Solid-State Nuclear Magnetic Resonance

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Hydration of Proteins: Excess Partial Volumes of Water and Proteins

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Water in Crystalline Fibers of Dihydrate β-Chitin Results in Unexpected Absence of Intramolecular Hydrogen Bonding

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The dynamic water vapour sorption properties of natural fibres and viscoelastic behaviour of the cell wall: is there a link between sorption kinetics and hysteresis?

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Insights into Hydrogen Bonding and Stacking Interactions in Cellulose

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A study of water exchange in wood by means of 2D NMR relaxation correlation and exchange

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Moisture changes in the plant cell wall force cellulose crystallites to deform

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Nanostructural assembly of cellulose, hemicellulose, and lignin in the middle layer of secondary wall of ginkgo tracheid

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Structure and properties of the cellulose microfibril

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IR and Raman spectra of liquid water: Theory and interpretation

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Hydration effects on spacing of primary-wall cellulose microfibrils:: a small angle X-ray scattering study

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Counterion condensation on charged spheres, cylinders, and planes

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JOURNAL OF PHYSICAL CHEMISTRY B (2007)

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Microfibril diameter in celery collenchyma cellulose:: X-ray scattering and NMR evidence

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Cellulose microfibril aggregates and their size variation with cell wall type

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Moisture uptake in native cellulose -: the roles of different hydrogen bonds:: a dynamic FT-IR study using Deuterium exchange

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Pore and matrix distribution in the fiber wall revealed by atomic force microscopy and image analysis

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Molecular conformations at the cellulose-water interface

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Characterization of the crystalline structure of cellulose using static and dynamic FT-IR spectroscopy

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Structural details of crystalline cellulose from higher plants

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BIOMACROMOLECULES (2004)

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Crystal structure and hydrogen bonding system in cellulose 1α, from synchrotron X-ray and neutron fiber diffraction

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Measurement of freezing point depression of water in glass capillaries and the associated ice front shape

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Crystal structure and hydrogen-bonding system in cellulose 1β from synchrotron X-ray and neutron fiber diffraction

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New insight into cellulose structure by atomic force microscopy shows the Iα crystal phase at near-atomic resolution

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