General Entropy Approach Toward Ultratough Sustainable Plastics.

Entropy is a universal concept across the physics of mixtures. While the role of entropy in other multicomponent materials has been appreciated, its effects in polymers and plastics have not. In this work, it is demonstrated that the seemingly small mixing entropy contributes to the miscibility and performance of polymer alloys. Experimental and modeling studies on over 30 polymer pairs reveal a strong correlation between entropy, morphology, and mechanical properties, while elucidating the mechanism behind: in polymer blends with weak interactions, entropy leads to homogeneously dispersed nanosized domains stabilized by highly entangled chains. This unique microstructure promotes uniform plastic deformation at the interface, thus improving the toughness of conventional brittle polymers by 1-2 orders of magnitude without sacrificing other properties, analogous to high-entropy metallic alloys. The proposed strategy also applies to ternary polymer systems and copolymers, offering a new pathway toward the development of sustainable polymers.

Entropically Toughened Robust Biodegradable Polymer Blends and Composites for Bone Tissue Engineering.

Biodegradable polymers and composites are promising candidates for biomedical implants in tissue engineering. However, state-of-the-art composite scaffolds suffer from a strength-toughness dilemma due to poor interfacial adhesion and filler dispersion. In this work, we propose a facile and scalable strategy to fabricate strong and tough biocomposite scaffolds through interfacial toughening. The immiscible biopolymer matrix is compatible by the direct incorporation of a third polymer. Densely entangled polymer chains lead to massive crazes and global shear yields under tension. Weak chemical interaction and high-shear melt processing create nanoscale dispersion of nanofillers within the matrix. The resultant ternary blends and composites exhibit an 11-fold increase in toughness without compromising stiffness and strength. At 70% porosity, three-dimensional (3D)-printed composite scaffolds demonstrate high compressive properties comparable to those of cancellous bones. In vitro cell culture on the scaffolds demonstrates not only good cell viability but also effective osteogenic differentiation of human mesenchymal stem cells. Our findings present a widely applicable strategy to develop high-performance biocomposite materials for tissue regeneration.