Low-Birefringent and Highly Tough Nanocellulose-Reinforced Cellulose Triacetate

Improvement of the mechanical and thermal properties of cellulose triacetate (CTA) films is required without sacrificing their optical properties. Here, poly(ethylene glycol) (PEG)-grafted cellulose nanofibril/CTA nanocomposite films were fabricated by casting and drying methods. The cellulose nanofibrils were prepared by 2,2,6,6-tetramethylpiperidine-1-oxyl (TEMPO)-mediated oxidation, and amine-terminated PEG chains were grafted onto the surfaces of the TEMPO-oxidized cellulose nanofibrils (TOCNs) by ionic bonds. Because of the nanosize effect of TOCNs with a uniform width of ∼3 nm, the PEG-TOCN/CTA nanocomposite films had high transparency and low birefringence. The grafted PEG chains enhanced the filler-matrix interactions and crystallization of matrix CTA molecules, resulting in the Young's modulus and toughness of CTA film being significantly improved by PEG-grafted TOCN addition. The coefficient of thermal expansion of the original CTA film was mostly preserved even with the addition of PEG-grafted TOCNs. These results suggest that PEG-TOCNs are applicable to the reinforcement for transparent optical films.