Abstract
Major challenge remains in the design and fabrication of artificial hierarchical materials that mimic the structural and functional features of these natural materials. Here, a novel biomimetic strategy to assemble hierarchical materials from biological nanobuilding blocks is demonstrated. The constituents and structures of the materials are designed by multiscale modeling and then experimentally constructed by multiscale self-assembly. The resultant materials that consist of silk nanofibrils (SNFs), hydroxyapatite (HAP), and chitin nanofibrils (CNFs) show nacre-like structures with mechanical strength and toughness better than most natural nacre and nacre-like nanocomposites. In addition, these SNF/HAP:CNF nanocomposites can be programmed into "grab-and-release" actuators due to the gradient structure of the nanocomposites as well as the high water sensitivity of each of the components, and thusshow potential applications in the design of novel third-generation biomaterials for potential clinical applications. In addition, this "in silico design and biomimetic assembly" route represents a rational, low-cost, and efficient strategy for the design and preparation of robust, hierarchical, and functional nanomaterials to meet a variety of application requirements in bio-nanotechnologies.
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