Control of Mechanical and Fracture Properties in Two-Phase Materials Reinforced by Continuous, Irregular Networks.

Composites with high strength and high fracture resistance are desirable for structural and protective applications. Most composites, however, suffer from poor damage tolerance and are prone to unpredictable fractures. Understanding the behavior of materials with an irregular reinforcement phase offers fundamental guidelines for tailoring their performance. Here, the fracture nucleation and propagation in two phase composites, as a function of the topology of their irregular microstructures is studied. A stochastic algorithm is used to design the polymeric reinforcing network, achieving independent control of topology and geometry of the microstructure. By tuning the local connectivity of isodense tiles and their assembly into larger structures, the mechanical and fracture properties of the architected composites are tailored at the local and global scale. Finally, combining different reinforcing networks into a spatially determined meso-scale assembly, it is demonstrated how the spatial propagation of fracture in architected composite materials can be designed and controlled a priori.

Extracting Geometry and Topology of Orange Pericarps for the Design of Bioinspired Energy Absorbing Materials.

As a result of evolution, many biological materials have developed irregular structures that lead to outstanding mechanical performances, like high stiffness-to-weight ratios and good energy absorption. However, reproducing these irregular biological structures in synthetic materials remains a complex design and fabrication challenge. Here, a bioinspired material design method is presented that characterizes the irregular structure as a network of building blocks, also known as tiles, and rules to connect them. Rather than replicating the biological structure one-to-one, synthetic materials are generated with the same distributions of tiles and connectivity rules as the biological material and it is shown that these equivalent materials have structure-to-property relationships similar to the biological ones. To demonstrate the method, the pericarp of the orange, a member of the citrus family known for its protective, energy-absorbing capabilities is studied. Polymer samples are generated and characterized under quasistatic and dynamic compression and display spatially-varying stiffness and good energy absorption, as seen in the biological materials. By quantifying which tiles and connectivity rules locally deform in response to loading, it is also determined how to spatially control the stiffness and energy absorption.

Hierarchical Porous Monoliths of Steel with Self-Reinforcing Adaptive Properties.

Porous structures offer an attractive approach to reduce the amount of natural resources used while maintaining relatively high mechanical efficiency. However, for some applications the drop in mechanical properties resulting from the introduction of porosity is too high, which has limited the broader utilization of porous materials in industry. Here, it is shown that steel monoliths can be designed to display high mechanical efficiency and reversible self-reinforcing properties when made with porous architectures with up to three hierarchical levels. Ultralight steel structures that can float on water and autonomously adapt their stiffness are manufactured by the thermal reduction and sintering of 3D printed foam templates. Using distinct mechanical testing techniques, image analysis, and finite element simulations, the mechanisms leading to the high mechanical efficiency and self-stiffening ability of the hierarchical porous monoliths are studied. The design and fabrication of mechanically stable porous monoliths using iron as a widely available natural resource is expected to contribute to the future development of functional materials with a more sustainable footprint.

Tough Bioinspired Composites That Self-Report Damage.

The increasing use of lightweight composite materials in structural applications requires the development of new damage monitoring technologies to ensure their safe use and prevent accidents. Although several molecular strategies have been proposed to report damage in polymers through mechanochromic responses, these approaches have not yet been translated into lightweight bioinspired composites for load-bearing applications. Here, we report on the development of bioinspired laminates of alternating polymer and nacre-like layers that combine optical translucency, high fracture toughness, and damage-reporting capabilities. The composites signal damage via a fluorescence color change that arises from the force activation of mechanophore molecules embedded in the material's polymer phase. A quantitative correlation between the applied strain and the fluorescence intensity was successfully established. We demonstrate that optical imaging of mechanically loaded composites allows for the localized detection of damage prior to fracture. This fluorescence-based self-reporting mechanism offers a promising approach for the early detection of damage in lightweight structural composites and can serve as a useful tool for the analysis of fracture processes in bulk transparent materials.

Fabrication of Three-Dimensional Polymer-Brush Gradients within Elastomeric Supports by Cu0-Mediated Surface-Initiated ATRP.

Cu0-mediated surface-initiated ATRP (Cu0 SI-ATRP) emerges as a versatile, oxygen-tolerant process to functionalize three-dimensional (3D), microporous supports forming single and multiple polymer-brush gradients with a fully tunable composition. When polymerization mixtures are dispensed on a Cu0-coated plate, this acts as oxygen scavenger and source of active catalyst. In the presence of an ATRP initiator-bearing microporous elastomer placed in contact with the metallic plate, the reaction solution infiltrates by capillarity through the support, simultaneously triggering the controlled growth of polymer brushes. The polymer grafting process proceeds with kinetics that are determined by the progressive infiltration of the reaction solution within the microporous support and by the continuous diffusion of catalyst regenerated at the Cu0 surface. The combination of these effects enables the accessible generation of 3D polymer-brush gradients extending across the microporous scaffolds used as supports, finally providing materials with a continuous variation of interfacial composition and properties.

Transparent and tough bulk composites inspired by nacre.

Materials combining optical transparency and mechanical strength are highly demanded for electronic displays, structural windows and in the arts, but the oxide-based glasses currently used in most of these applications suffer from brittle fracture and low crack tolerance. We report a simple approach to fabricate bulk transparent materials with a nacre-like architecture that can effectively arrest the propagation of cracks during fracture. Mechanical characterization shows that our glass-based composites exceed up to a factor of 3 the fracture toughness of common glasses, while keeping flexural strengths comparable to transparent polymers, silica- and soda-lime glasses. Due to the presence of stiff reinforcing platelets, the hardness of the obtained composites is an order of magnitude higher than that of transparent polymers. By implementing biological design principles into glass-based materials at the microscale, our approach opens a promising new avenue for the manufacturing of structural materials combining antagonistic functional properties.