Mechanically strong and biodegradable holocellulose films prepared from Camellia oleifera shells

Bioplastic derived from renewable lignocellulosic biomass is an attractive alternative to petroleum-based plastics. Herein, Callmellia oleifera shells (COS), a unique byproduct from tea oil industry, were delignified and converted into high-performance bio-based films via a green citric acid treatment (15 %, 100 °C and 24 h), taking advantage of their high hemicellulose content. The structure-property relations of COS holocellulose (COSH) films were systematically analyzed considering different treatment conditions. The surface reactivity of COSH was improved via a partial hydrolysis route and strong hydrogen bonding formed between the holocellulose micro/nanofibrils. COSH films exhibited high mechanical strength, high optical transmittance, improved thermal stability, and biodegradability. A mechanical blending pretreatment of COSH, which disintegrated the COSH fibers before the citric acid reaction, further enhanced the tensile strength and Young's modulus of the films up to 123.48 and 5265.41 MPa, respectively. The films decomposed completely in soil, demonstrating an excellent balance between degradability and durability.