Cellulose nanocrystal-coated TEMPO-oxidized cellulose nanofiber films for high performance all-cellulose nanocomposites

High performance biopolymer films are of great interest as effective alternatives to non-biodegradable and petroleum-based polymer films. However, most natural biopolymer films possess weak mechanical and poor gas barrier properties, limiting their applicability. In this work, we developed all-cellulose nanocomposite films through a simple vacuum filtration process, using cellulose nanocrystals (CNCs) and 2,2,6,6-tetramethylpiperidine-1-oxy-oxidized cellulose nanofibers (TEMPO-CNFs). The TEMPO-CNFs were employed to construct a transparent, free-standing substrate matrix and the CNCs were used as a coating material to improve the mechanical and water vapor barrier properties of the final material. We have demonstrated that the top and bottom CNCs-coated TEMPO-CNF substrates (CNC/TEMPO-CNF/CNC) have excellent mechanical and good water vapor barrier properties. The resulting CNC/TEMPO-CNF/CNC films revealed a high tensile strength of 114 MPa and a low specific water vapor transmission rate (SWVTR) of 19 g∙mm/m2∙day. In addition, the CNC/TEMPO-CNF/CNC films were resistant to various solvents including water, ethanol, tetrahydrofuran (THF), and acetone. This type of high performance cellulose nanocomposite can be used as a renewable material for a broad range of potential applications.