Hydrogen Bond‐Mediated Strong Plasticization for High‐Performance Alginate Plastics

The increasingly severe plastic pollution has urged an inevitable trend to develop biodegradable plastic products that can take over synthetic plastics. As one of the most abundant natural polymers, polysaccharides are an ideal candidate to substitute synthetic plastics. The rigidity of polysaccharide chains principally allows for high strength and stiffness of their materials, however, challenges the facile orientation in material processing. Here, a general hydrogen bond-mediated plasticization strategy to regulate isotropic sodium alginate (SA) chains to a highly ordered state is developed, and alginate plastics with high performances are fabricated. It is revealed that hydroxyl groups in glycerol modulate the viscoelasticity of SA solids by forming strong hydrogen bonds with SA chains, achieving a large stretchability at a high solid content. Highly orientated alginate films exhibit a superior tensile strength of 575 MPa and toughness of 60.7 MJ m^-3, outperforming most regenerated biomass films. The high solid content and large stretchability mediated by strong hydrogen bonding ensure plastic molding of solid-like SA with high fidelity. This hydrogen bond-mediated plasticity provides a facile but effective method to justify the high performances of polysaccharide-based plastics.