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In this work, deep eutectic solvent (DES) based on imidazole and triethylmethylammonium chloride was used as a reaction medium for the esterification of cellulose nanofiber (CNF) and all-cellulose composite (ACC) films with n-octylsuccinic anhydride (OSA) to obtain high strength and sustainable films with increased hydrophobicity. Diffuse reflectance infrared Fourier transform spectroscopy and X-ray photoelectron spectroscopy were used to prove the success of the modification. The mechanical strength of the modified films was analyzed in dry, humid, and wet conditions, and the hydrophobicity of the films was indicated in terms of contact angle measurements. In addition, water absorption and transparency of the films were characterized. The modification was proven to be simple and fast, and mild conditions of 80 °C reaction temperature and 1 h reaction time were used. DES/OSA- modified CNF film exhibited better mechanical properties in dry, humid, and wet conditions compared to reference CNF film, and DES/OSA-modified ACC film displayed notable higher mechanical properties in wet state compared to that of reference CNF film (31 MPa tensile strength and 6.1% strain at break vs. 18 MPa and 2.2%, respectively). These improvements were partly attributed to higher contact angles of modified films (ACC-DES/OSA 60° and CNF-DES/OSA 51°) compared to CNF film (37°). Graphic abstract

Hydrophobic modification of nanocellulose and all-cellulose composite films using deep eutectic solvent as a reaction medium