Computational modeling of the structure relaxation and dispersion thermodynamics of pristine and modified cellulose nanocrystals in solution

Cellulose nanocrystals (CNC) exhibit superior mechanical properties and attracted attention as reinforcing additives in polymer nanocomposites. Large-scale use of CNC in polymer and biocomoposite materials is currently limited due to its low solubility in nonpolar solvents. We employ a multiscale modeling platform based on the 3D-RISM-KH molecular theory of solvation to study the solvation structure and effective interactions of pristine, sulfonated, and esterified CNC in water, aqueous NaCl solution, an ionic liquid, and benzene. Insights from these studies are intended to help rationally design grafted CNC particles with improved dispersion and preserved mechanical properties that can be more effectively incorporated into materials as reinforcement additives.