Bioinspired Design of Strong, Tough, and Thermally Stable Polymeric Materials <i>via</i> Nanoconfinement

The combination of high strength, great toughness, and high heat resistance for polymeric materials is a vital factor for their practical applications. Unfortunately, until now it has remained a major challenge to achieve this performance portfolio because the mechanisms of strength and toughness are mutually exclusive. In the natural world, spider silk features the combination of high strength, great toughness, and excellent thermal stability, which are governed by the nanoconfinement of hydrogen-bonded β-sheets. Here, we report a facile bioinspired methodology for fabricating advanced polymer composite films with a high tensile strength of 152.8 MPa, a high stiffness of 4.35 GPa, and a tensile toughness of 30.3 MJ/m3 in addition to high thermal stability (69 °C higher than that of the polymer matrix) only by adding 2.0 wt % of artificial β-sheets. The mechanical and thermostable performance portfolio is superior to that of its counterparts developed to date because of the nanoconfinement and hydrogen-bond cross-linking effects of artificial β-sheets. Our study offers a facile biomimetic strategy for the design of integrated mechanically robust and thermostable polymer materials, which hold promise for many applications in electrical devices and tissue engineering fields