Massively Preparable, Super-tough and Ultra-strong Cellulose-based Bioplastics Enabled by Microphase Separation

Abstract The growing environmental concern over petroleum-based plastics have promoted the exploration of sustainable bioplastics with competitive properties. Cellulose is an ideal sustainable alternative with endless sources and biodegradability, but poor processability and poor toughness severely restrict their practical applications. Herein, a microphase separation strategy is proposed to massively prepare super-tough and ultra-strong cellulosic plastics. The microphase separation is realized by thermoplastic processing and water-soaking process, highlighting the potential of large-scale preparation. The combined microphases (100 ~ 300 nm) and rigid continuous phase enable a tensile strength of 147.6 ± 9.6 MPa and a toughness of 30.2 ± 2.1 MJ/m³, where numerous microphases play a unique toughening role via forcing the movement of rigid chain-segments. Besides, the microphase-separated cellulosic plastics possess excellent UV-shielding effect, good transparency, high glass transition temperature, high decomposition temperature and good solvent resistance, stressing the excellent comprehensive properties and wide applicability. The combined large-scale preparation and excellent comprehensive properties are unprecedented for cellulosic plastics. This work provides a novel yet facile microphase separation strategy to prepare high-performance cellulosic plastics, and will promote the substitution of petroleum-based plastics by sustainable cellulosic plastics with endless sources.