Toward millimeter thick cellulose nanofiber/epoxy laminates with good transparency and high flexural strength.

While cellulose nanofiber-based bioplastics are of great interest for replacing synthetic polymer and glass materials, the main limitation is their low thickness, which makes them difficult for various applications. In this study, we fabricated millimeter-scale thick bioplastic composites, based on 2,2,6,6-tetramethylpiperidine-1-oxy-oxidized cellulose nanofibers (TEMPO-CNF) and epoxy resin, via sequential lamination processes. The glycerol as softener was added to TEMPO-CNF dispersion to prepare a thick TEMPO-CNF layer without shrinkage. It was discovered that the total thickness of TEMPO-CNF/epoxy laminates can be easily controlled by changing the thickness and number of TEMPO-CNF layers and the total thickness can also be easily increased up to 2.4 mm. Furthermore, these TEMPO-CNF/epoxy laminates have high flexural strength (272 MPa) as well as good transmittance (85% % at 600 nm). We anticipate that our approach will significantly broaden the strategies for fabricating nanocellulose-based bioplastics for use as a replacement for transparent synthetic polymers and glass materials.