Bottom-Up Film-to-Bulk Assembly Toward Bioinspired Bulk Structural Nanocomposites.

Biological materials, although composed of meager minerals and biopolymers, often exhibit amazing mechanical properties far beyond their components due to hierarchically ordered structures. Understanding their structure-properties relationships and replicating them into artificial materials would boost the development of bulk structural nanocomposites. Layered microstructure widely exists in biological materials, serving as the fundamental structure in nanosheet-based nacres and nanofiber-based Bouligand tissues, and implying superior mechanical properties. High-efficient and scalable fabrication of bioinspired bulk structural nanocomposites with precise layered microstructure is therefore important yet remains difficult. Here, one straightforward bottom-up film-to-bulk assembly strategy is focused for fabricating bioinspired layered bulk structural nanocomposites. The bottom-up assembly strategy inherently offers a methodology for precise construction of bioinspired layered microstructure in bulk form, availability for fabrication of bioinspired bulk structural nanocomposites with large sizes and complex shapes, possibility for design of multiscale interfaces, feasibility for manipulation of diverse heterogeneities. Not limited to discussing what has been achieved by using the current bottom-up film-to-bulk assembly strategy, it is also envisioned how to promote such an assembly strategy to better benefit the development of bioinspired bulk structural nanocomposites. Compared to other assembly strategies, the highlighted strategy provides great opportunities for creating bioinspired bulk structural nanocomposites on demand.

Bioinspired polysaccharide-based nanocomposite membranes with robust wet mechanical properties for guided bone regeneration.

Polysaccharide-based membranes with excellent mechanical properties are highly desired. However, severe mechanical deterioration under wet conditions limits their biomedical applications. Here, inspired by the structural heterogeneity of strong yet hydrated biological materials, we propose a strategy based on heterogeneous crosslink-and-hydration (HCH) of a molecule/nano dual-scale network to fabricate polysaccharide-based nanocomposites with robust wet mechanical properties. The heterogeneity lies in that the crosslink-and-hydration occurs in the molecule-network while the stress-bearing nanofiber-network remains unaffected. As one demonstration, a membrane assembled by bacterial cellulose nanofiber-network and Ca2+-crosslinked and hydrated sodium alginate molecule-network is designed. Studies show that the crosslinked-and-hydrated molecule-network restricts water invasion and boosts stress transfer of the nanofiber-network by serving as interfibrous bridge. Overall, the molecule-network makes the membrane hydrated and flexible; the nanofiber-network as stress-bearing component provides strength and toughness. The HCH dual-scale network featuring a cooperative effect stimulates the design of advanced biomaterials applied under wet conditions such as guided bone regeneration membranes.

Scalable Manufacturing of Mechanical Robust Bioinspired Ceramic-Resin Composites with Locally Tunable Heterogeneous Structures.

Lightweight structural materials with a unique combination of high stiffness, strength, toughness, and hardness, are highly desired yet challenging to be artificially fabricated. Biological structural materials, on the other hand, ingeniously integrate multiple mutually exclusive mechanical properties together relying on their hierarchically heterogeneous structures bonded with gradient interfaces. Here, a scalable bottom-up approach combining continuous nanofiber-assisted evaporation-induced self-assembly with laminating, pressure-less sintering and resin infiltration is reported to fabricate bioinspired heterogeneous ceramic-resin composites with locally tunable microstructure to fulfill specific properties. A gradient interlayer is introduced to provide a gradual transition between adjacent heterogeneous layers, effectively alleviating their property mismatch. The optimized heterogeneous nacre-like composite, as a demonstration, exhibits an attractive combination of low density (≈2.8 g cm-3 ), high strength (≈292 MPa), toughness (≈6.4 MPa m1/2 ), surface hardness (≈1144 kgf mm-2 ) and impact-resistance, surpassing the overall performance of engineering alumina. This material-independent approach paves the way for designing advanced bioinspired heterogeneous materials for diverse structural and functional applications.

Bioinspired Impact-Resistant and Self-Monitoring Nanofibrous Composites.

Lightweight and impact-resistant materials with self-monitoring capability are highly desired for protective applications, but are challenging to be artificially fabricated. Herein, a scalable-manufactured aramid nanofiber (ANF)-based composite combining these key properties is presented. Inspired by the strengthening and toughening mechanisms relying on recoverable interfaces commonly existing in biological composites, mechanically weak but dense hydrogen bonds are introduced into the ANF interfaces to achieve simultaneously enhanced tensile strength (300 MPa), toughness (55 MJ m-3 ), and impact resistance of the nanofibrous composite. The achieved mechanical property combination displays attractive advantages compared with that of most of previously reported nanocomposites. Additionally, the nanofibrous composite is designed with a capability for real-time self-monitoring of its structural safety during both quasi-static tensile and dynamic impact processes, based on the strain/damage-induced resistance variations of a conductive nanowire network inside it. These comprehensive properties enable the present nanofibrous composite with promising potential for protective applications.