Abstract

The transition toward renewable and environmentally responsible materials has intensified interest in cellulose-based systems for use in sustainable packaging applications. Although cellulose offers biocompatibility, structural versatility, and tuneable physicochemical properties, conventional modification routes rely on harsh chemicals and generate environmentally burdensome effluents. In this study, an efficient and a potentially green strategy for cellulose modification was developed using acid-based deep eutectic solvents (DES) composed of choline chloride and lactic, acetic, or citric acid at different molar ratios. Under mild conditions (110 °C, 4 h), DES pretreatment reduced glucan content in sulphite pulp from 99% to 79–93%, depending on the hydrogen bond donor (HBD), while suggesting an apparent increase in relative crystallinity, from approximately 82% to 90%, as estimated by the Segal method. FTIR, XRD, and morphological analyses revealed the disruption of the hydrogen bonding network, enhanced fibrillation, and residual DES-derived functional groups detectable by FTIR. Although DES pretreatment increased structural order, it also reduced enzymatic digestibility due to the higher proportion of crystalline domains. Overall, the results demonstrate that acidic DES constitutes a sustainable and recyclable medium capable of modulating cellulose structure and generating materials with enhanced physicochemical properties. These findings suggest that DES-modified cellulose could serve as a potential reinforcement platform for future biodegradable packaging and bioplastic formulations, enabling the development of high-performance, renewable, and environmentally compliant packaging materials.

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