A robust strategy for thermoformable cellulosic composite bioplastics <i>via</i> hydrogen bond substitution

Cellulose represents a promising renewable resource for the development of sustainable alternatives to petroleum-derived plastics, owing to its exceptional biodegradability and renewability. However, the extensive hydrogen-bonding network and ordered crystalline structure of cellulose limit its solubility and thermo-processability, posing significant challenges for large-scale production of recyclable high-performance bioplastics. In this study, we propose a robust strategy for cellulosic composite bioplastic by controlling the disruption and reformation of hydrogen bonds in ethyl cellulose (EC) nanocomposites incorporating rheologically tunable graphene (Rt-G), which can dynamically dissociate hydrogen bonds within the EC matrix. The cellulosic composite bioplastic can be efficiently formed <i>via</i> mild thermal processing at 150 °C under 20 MPa for 1 hour, demonstrating good thermoplastic processability across multiple cycles of thermoplastic processing and recovery molding. In addition, the cellulose composite bioplastic demonstrate approximately fivefold enhancements in both toughness and thermal conductivity compared to those of pristine EC. And they can be repeatedly reprogrammed into diverse shapes under mild processing conditions through thermoplasticity induced by hydrogen-bond disruption and reformation. These findings provide a promising pathway for the development of high-performance cellulosic composite bioplastics, offering a viable alternative to conventional petroleum-derived plastics.