A critical review of all-cellulose composites

Cellulose is a fascinating biopolymer of almost inexhaustible quantity. While being a lightweight material, it shows outstanding values of strength and stiffness when present in its native form. Unsurprisingly, cellulose fibre has been rigorously investigated as a reinforcing component in biocomposites. In recent years, however, a new class of monocomponent composites based on cellulosic materials, so-called all-cellulose composites (ACCs) have emerged. These new materials promise to overcome the critical problem of fibre–matrix adhesion in biocomposites by using chemically similar or identical cellulosic materials for both matrix and reinforcement. A number of papers scattered throughout the polymer, composites and biomolecular science literature have been published describing non-derivatized and derivatized ACCs. Exceptional mechanical properties of ACCs have been reported that easily exceed those of traditional biocomposites. Several different processing routes have been applied to the manufacture of ACCs using a broad range of different solvent systems and raw materials. This article aims to provide a comprehensive review of the background chemistry and various cellulosic sources investigated, various synthesis routes, phase transformations of the cellulose, and mechanical, viscoelastic and optical properties of ACCs. The current difficulties and challenges of ACCs are clearly outlined, pointing the way forward for further exploration of this interesting subcategory of biocomposites.