Energy consumption and post-treatment of chemical reagent residues are important issues that hinder the sustainable production of the natural building blocks of cellulose nanofibrils (CNFs). In this study, we realize a low-energy, zero-waste process for CNF production by designing a novel reactive deep eutectic solvent (DES), the residue of which can be directly used as a plant growth regulator. After pretreatment with the DES, cellulose fibers self-delaminate into thin layers referred to as pseudo-CNFs, as their strength, toughness and transmittance are comparable to those of CNFs. Pseudo-CNFs break into smaller particles during recycling and thus display unique mechanical upcycling. After facile fibrillation, the obtained CNFs can independently form freestanding sub-micrometer films that show a strong, full coloration, which is demonstrated for the first time. Our concept can enable a green process, and the developed cellulosic materials may find various applications as structural materials and optical coatings.
Keywords: cellulose; deep eutectic solvent; full coloration; upcycling; zero waste.