Self-assembled optically transparent cellulose nanofibril films: effect of nanofibril morphology and drying procedure

Cellulose nanofibril (CNF) films currently provide great opportunity in many applications with advantages of excellent mechanical strength, high light transmittance, and good barrier properties. However, processes for preparing CNFs are typically tedious and vary, along with their properties. Here, five preparation methods using various combinations of filtration, freeze-drying, and casting are applied to produce CNF films, and their major properties are compared. Three different types of CNFs having a range of fiber diameter and aspect ratio were examined using each of these five preparation methods. Because of limited hydrogen bonds and nanofibril arrangement, the freeze-dried CNF films displayed reduced mechanical strength and light transmittance compared to the other methods, although freeze-drying was relatively fast. Some effects of film production methods on measured crystallinity were also observed with freeze-dried samples having lower crystallinity than films similarly produced by filtration and drying. Free-standing CNF films produced by casting at room temperature required long times and mold growth was sometimes observed, but cast films made from 2,2,6,6-tetramethylpiperidine-1-oxyl radical-oxidized CNFs had the highest light transmittance of any samples. Filtration of CNF suspensions followed by air- or oven-drying produced films with minimal defects, high mechanical strength, and good light transmittance with relatively little effort. Therefore, this filtration procedure is recommended for producing CNF films.