Solvent-Mediated Control of Nanocellulose Dispersion: An Integrated Computational and Experimental Investigation

Area of Science:

• Materials Science
• Biomaterials Engineering
• Computational Chemistry

Background:

• Fibrillated cellulose, including cellulose nanofibers (CNFs), offers a renewable, high-strength material for circular bioeconomies.
• Irreversible aggregation of nanocellulose architectures hinders practical applications.
• Solvent-based dispersion is a promising strategy to prevent CNF aggregation.

Purpose of the Study:

• To investigate how solvent environments influence cellulose nanofiber (CNF) interactions and dispersion stability.
• To establish a rational framework for solvent selection to achieve stable CNF dispersions.
• To enable the development of high-strength biobased materials and efficient bioenergy conversion.

Main Methods:

• Integrated classical and enhanced sampling molecular dynamics (MD) simulations.
• Experimental suspension rheology and atomic force microscopy (AFM).
• Liquid cell AFM imaging.

Main Results:

• Computed CNF-CNF contact free energies indicated reduced aggregation in specific solvents (e.g., acetone/water, GVL/water, THF/water, pure acetone) compared to pure water.
• CNF suspensions in these solvents showed stronger inter-fibril network structures and enhanced recovery, signifying improved CNF-solvent affinity.
• AFM imaging confirmed the presence of well-dispersed CNFs in selected solvent systems.

Conclusions:

• Solvent choice significantly impacts CNF aggregation and dispersion stability.
• A multiscale computational and experimental approach provides a framework for designing effective solvent systems for nanocellulose.
• This research facilitates the creation of advanced biobased materials and efficient bioenergy applications.