A Bioinspired Ultratough Composite Produced by Integration of Inorganic Ionic Oligomers within Polymer Networks

The nacre-inspired laminates are promising materials for their excellent mechanics. However, the interfacial defects between organic–inorganic phases commonly lead to the crack propagation and fracture failure of these materials under stress. A natural biomineral, bone, has much higher bending toughness than the nacre. The small size of inorganic building units in bone improves the organic–inorganic interaction, which optimizes the material toughness. Inspired by these biological structures, here, an ultratough nanocomposite laminate is prepared by the integration of ultrasmall calcium phosphate oligomers (CPO, 1 nm in diameter) within poly­(vinyl alcohol) (PVA) and sodium alginate (Alg) networks through a simple three-step strategy. Owing to the small size of inorganic building units, strong multiple molecular interactions within integrated organic–inorganic hierarchical structure are built. The resulting laminates exhibit ultrahigh bending strain (>50% without fracture) and toughness (21.5–31.0 MJ m^–3), which surpass natural nacre and almost all of the synthetic laminate materials that have been reported so far. Moreover, the mechanics of this laminate is tunable by changing the water content within the bulk structure. This work provides a way for the development of organic–inorganic nanocomposites with ultrahigh bending toughness by using inorganic ionic oligomers, which can be useful in the fields of tough protective materials and energy absorbing materials.