A new 3D printing strategy by enhancing shear-induced alignment of gelled nanomaterial inks resulting in stronger and ductile cellulose films.

Cellulose nanofibrils (CNFs) are derived from biomass and have significant potential as fossil-based plastic alternatives used in disposable electronics. Controlling the nanostructure of fibrils is the key to obtaining strong mechanical properties and high optical transparency. Vacuum filtration is usually used to prepare the CNFs film in the literature; however, such a process cannot control the structure of the CNFs film, which limits the transparency and mechanical strength of the film. Here, direct ink writing (DIW), a pressure-controlled extrusion process, is proposed to fabricate the CNFs film, which can significantly harness the alignment of fibrils by exerting shear stress force on the filaments. The printed films by DIW have a compact structure, and the degree of fibril alignment quantified by the small angle X-ray diffraction (SAXS) increases by 24 % compared to the vacuum filtration process. Such a process favors the establishment of the chemical bond (or interaction) between molecules, therefore leading to considerably high tensile strength (245 ± 8 MPa), elongation at break (2.2 ± 0.5 %), and good transparency. Thus, proposed DIW provides a new strategy for fabricating aligned CNFs films in a controlled manner with tunable macroscale properties. Moreover, this work provides theoretical guidance for employing CNFs as structural and reinforcing materials to design disposable electronics.