A multiple physical crosslinked cellulose-based bioplastics with robust mechanical and thermal stability.

The widespread use of traditional petroleum-based plastics has created an environmental crisis and health hazard, so there is an urgent need for bioplastics with excellent performance. However, fabricating of robust mechanical properties and heat resistance bioplastics in an efficient way has remained an enormous challenge. Herein, we proposed a strategy for the synergistic preparation of high-performance bioplastics with multiple physical crosslinking network structures via noncovalent and coordination bonds. In this strategy, carboxylated cellulose nanofibers (CNFs) and the polyphenol structures of tannic acid (TA) interacted noncovalently to create network structures; the bioplastic immersed in Ca solution formed ionic crosslinked networks and TA-Ca coordination bonds. The synergistic effect of multiple network structures composed of hydrogen and coordination bonds made cellulose-based bioplastics have dense structures and robust tensile strength (114.2 MPa), while bioplastics had the characteristics of high transparency and superior thermal stability. Furthermore, the laminated composites formed by the bioplastic and PVA could support 1,000 g easily, which allowed it to be used as weighing application. Thus, the proposed multiple physical crosslinking strategy provides a method for developing cellulose-based bioplastics with excellent performance, which offers a new approach for the subsequent development of sustainable green materials.