Thermostable and Redispersible Cellulose Nanocrystals with Thixotropic Gelation Behavior by a Facile Desulfation Process

As a ecofriendly and promising nanomaterial, cellulose nanocrystals (CNCs) have attracted significant interest. However, the intrinsic sulfate-modified surface and self-aggregation behavior of the most common acid-hydrolyzed CNCs with sulfuric acid lead to the low thermostability and poor redispersion of solid-state CNCs materials, which limit their practical applications. In this work, we propose a simple and effective strategy to not only remove the sulfates in CNCs but also resuscitate their dispersibility by a facile post-treatment process, including an acid-triggering gelation, solvent exchange with ethanol, and supercritical CO2 drying. The resultant CNC powder exhibits a high thermostability, much higher than that of the common acid-hydrolyzed CNCs and similar to that of the pristine cellulose. Moreover, the CNC powder can be readily redispersed in various solvents by a short ultrasonic treatment. Subsequently, as the CNC concentration increases, CNC gels spontaneously form and exhibit thixotropic behaviors. Taking advantage of these characteristics of the above desulfated CNC powder, we fabricated a CNC/Ag nanoparticle gel, magnetic CNC/Fe3O4 nanoparticle gel, pressure-sensitive polymer/CNC composite gel, and colorless and transparent poly(lactic acid)/CNC thermoplastic films. Therefore, the highly thermostable, redispersible, and easy-to-gel CNC powder has a huge potential as a building block for various stable, well-dispersed, and functional nanocomposite materials.