Hazelnut Shell Biorefinery for Bioactive CMC Films: Sequential Polyphenol and Cellulose Recovery and Wax-Modulating Performance

The valorization of lignocellulosic residues into bioactive and biodegradable materials offers a sustainable route for functional food packaging. In this study, hazelnut shells were exploited through an integrated process enabling the integrated recovery of polyphenols and cellulose. Polyphenols were extracted via hot water, liquid–liquid partitioning, and column chromatography, yielding a purified bioactive fraction. The residual biomass after polyphenol recovery was used for cellulose extraction (approximately 23% w/w) and converted into carboxymethyl cellulose (CMC) with a degree of substitution (DS) of 0.77. Active CMC films incorporating polyphenolic extracts exhibited improved mechanical performance, reaching tensile strengths of about 78 MPa and elongation at break values above 20%, while reducing water solubility to approximately 31%. The addition of carnauba wax further enhanced water resistance while modulating flexibility and stiffness. Attenuated Total Reflectance-Fourier Transform Infrared spectroscopy (ATR-FTIR) and scanning electron microscopy (SEM) analyses confirmed the conversion of crystalline cellulose into amorphous CMC and the successful incorporation of additives within the polymer matrix. The resulting films showed tunable mechanical, optical, and barrier properties, along with UV-blocking and antioxidant activity. These findings demonstrate that hazelnut shell-derived CMC films enriched with polyphenols and carnauba wax represent promising candidates for a sustainable platform for active food packaging applications, supporting a circular waste-to-value approach.