Critical-Like Gelation Dynamics in Cellulose Nanocrystal Suspensions.

Abstract

We use time-resolved mechanical spectroscopy to offer a detailed picture of the gelation dynamics of cellulose nanocrystal (CNC) suspensions following shear cessation in the presence of salt. CNCs are charged, rodlike colloids that self-assemble into various phases, including physical gels serving as soft precursors for biosourced composites. Here, a series of linear viscoelastic spectra acquired across the sol-gel transition of CNC suspensions are rescaled onto two master curves that correspond to a viscoelastic liquid state prior to gelation and to a soft solid state after gelation. These two states are separated by a critical gel point, where all rescaling parameters diverge in an asymmetric fashion yet with exponents that obey hyperscaling relations consistent with previous works on isotropic colloids and polymer gels. Upon varying the salt content, we further show that these critical-like dynamics result in both time-connectivity and time-concentration superposition principles.