Surface modification effects on nanocellulose – molecular dynamics simulations using umbrella sampling and computational alchemy

Chen, Pan; Re, Giada Lo; Berglund, Lars A.; Wohlert, Jakob

doi:10.1039/d0ta09105g

Cited by 32 publications

(26 citation statements)

References 66 publications

(64 reference statements)

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“…Water is shown in light blue. Reproduced from Chen et al (2020) with permission from the Royal Society of Chemistry Fibril-fibril aggregation and hornification Fibrils both in suspension and in the plant cell wall form self-associated structures. However, under ambient conditions fibrils in plant cell walls do not fuse completely to form larger crystallites, which makes them distinguishable as separate entities using experimental methods such as X-ray and neutron scattering (Jarvis 2018).…”

Section: Adsorption To Cellulosementioning

confidence: 99%

“…Wherever the molecular structure prevents a perfect fit between fibrils, such as anti-parallel arrangement (Chen et al 2019), fibril twist (Paajanen et al 2019), adsorbed hemicelluloses (Thomas et al 2020) or the presence of a chemically modified surface (Chen et al 2020), small sub-nano-sized cavities are present, which can harbor water molecules (Fig. 6).…”

Section: Adsorption To Cellulosementioning

confidence: 99%

“…The extent of hornification depends strongly on drying methods (Peng et al 2012; Nodenstro ¨m 2020) and can also be mitigated by additives such as glycerol (Moser et al 2018), which presumably act as spacers between fibrils. It also depends on surface chemistry of the fibrils (Benselfelt et al 2019), where for instance acetylation was shown to reduce the work of adhesion between fibrils in water (Chen et al 2020) due to the surface acetyl groups preventing tight association leading to the interpenetration of water molecules at the interface (Fig. 6).…”

Section: Adsorption To Cellulosementioning

confidence: 99%

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

Bergenstråhle-Wohlert

et al. 2021

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In the cellulose scientific community, hydrogen bonding is often used as the explanation for a large variety of phenomena and properties related to cellulose and cellulose based materials. Yet, hydrogen bonding is just one of several molecular interactions and furthermore is both relatively weak and sensitive to the environment. In this review we present a comprehensive examination of the scientific literature in the area, with focus on theory and molecular simulation, and conclude that the relative importance of hydrogen bonding has been, and still is, frequently exaggerated.

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Section: Adsorption To Cellulosementioning

confidence: 99%

Section: Adsorption To Cellulosementioning

confidence: 99%

Section: Adsorption To Cellulosementioning

confidence: 99%

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

Bergenstråhle-Wohlert

et al. 2021

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“…This protocol was recently used for simulations of acetylated cellooligomers and cellulose nanocrystals. 52 …”

Section: Methodsmentioning

confidence: 99%

O-Methylation in Carbohydrates: An NMR and MD Simulation Study with Application to Methylcellulose

2021

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Methylated carbohydrates are important from both biological and technical perspectives. Specifically, methylcellulose is an interesting cellulose derivative that has applications in foods, materials, cosmetics, and many other fields. While the molecular dynamics simulation technique has the potential for both advancing the fundamental understanding of this polymer and aiding in the development of specific applications, a general drawback is the lack of experimentally validated interaction potentials for the methylated moieties. In the present study, simulations using the GROMOS 56 carbohydrate force field are compared to NMR spin–spin coupling constants related to the conformation of the exocyclic torsion angle ω in d -glucopyranose and derivatives containing a 6-O-methyl substituent and a 13 C-isotopologue thereof. A 3 J CC Karplus-type relationship is proposed for the C5–C6–O6–C Me torsion angle. Moreover, solvation free energies are compared to experimental data for small model compounds. Alkylation in the form of 6-O-methylation affects exocyclic torsion only marginally. Computed solvation free energies between nonmethylated and methylated molecules were internally consistent, which validates the application of these interaction potentials for more specialized purposes.

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“…The details of the molecular docking of the enzyme-substrate complex would be helpful to optimize the overall economics of processing lignocellulosic materials in the production of NC [ 18 ]. After that, the surface chemistry of NC could be further altered (with the aid of MDS) to improve their dispersibility in on-polar polymers [ 19 ]. Coarse-grained modelling was greatly utilized in biomolecular systems that involve mainly carbohydrates, where the number of atoms or molecules were reduced into a single bead to interact with other pre-defined beads in a dynamic system.…”

Section: Introductionmentioning

confidence: 99%

Molecular Dynamics Simulation of Nanocellulose-Stabilized Pickering Emulsions

et al. 2021

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While the economy is rapidly expanding in most emerging countries, issues coupled with a higher population has created foreseeable tension among food, water, and energy. It is crucial for more sustainable valorization of resources, for instance, nanocellulose, to address the core challenges in environmental sustainability. As the complexity of the system evolved, the timescale of project development has increased exponentially. However, research on the design and operation of integrated nanomaterials, along with energy supply, monitoring, and control infrastructure, has seriously lagged. The development cost of new materials can be significantly reduced by utilizing molecular simulation technology in the design of nanostructured materials. To realize its potential, nanocellulose, an amphiphilic biopolymer with the presence of rich -OH and -CH structural groups, was investigated via molecular dynamics simulation to reveal its full potential as Pickering emulsion stabilizer at the molecular level. This work has successfully quantified the Pickering stabilization mechanism profiles by nanocellulose, and the phenomenon could be visualized in three stages, namely the initial homogenous phase, rapid formation of micelles and coalescence, and lastly the thermodynamic equilibrium of the system. It was also observed that the high bead order was always coupled with a high volume of phase separation activities, through a coarse-grained model within 20,000 time steps. The outcome of this work would be helpful to provide an important perspective for the future design and development of nanocellulose-based emulsion products, which cater for food, cosmeceutical, and pharmaceutical industries.

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Surface modification effects on nanocellulose – molecular dynamics simulations using umbrella sampling and computational alchemy

Abstract: Topochemical modification of nanocellulose particles, in particular acetylation, is commonly used to reduce hygroscopicity and improve dispersibility in polymers. Despite enormous experimental efforts on cellulose surface modification, there is currently...

Cited by 32 publications

References 66 publications

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

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

O-Methylation in Carbohydrates: An NMR and MD Simulation Study with Application to Methylcellulose

Molecular Dynamics Simulation of Nanocellulose-Stabilized Pickering Emulsions

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