Critical-like gelation dynamics in cellulose nanocrystal suspensions

TL;DR

This study investigates the gelation process of cellulose nanocrystal suspensions using mechanical spectroscopy, revealing critical-like dynamics and superposition principles near the gel point influenced by salt content.

Contribution

It provides a detailed characterization of the gelation dynamics of CNC suspensions, identifying critical-like behavior and superposition principles that depend on salt concentration.

Findings

Identification of a critical gel point with diverging parameters

Observation of asymmetric divergence consistent with hyperscaling

Demonstration of time-connectivity and time-concentration superposition

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.