Anisotropic hydrogels with a hierarchical structure can mimic biological tissues, such as neurons or muscles that show directional functions, which are important factors for signal transduction and cell guidance. Here, we report a mussel-inspired approach to fabricate an anisotropic hydrogel based on a conductive ferrofluid. First, polydopamine (PDA) was used to mediate the formation of PDA-chelated carbon nanotube-Fe3O4 (PFeCNT) nanohybrids and also used as a dispersion medium to stabilize the nanohybrids to form a conductive ferrofluid. The ferrofluid can respond to an orientated magnetic field and be programed to form aligned structures, which were then frozen in a hydrogel network formed via in situ free-radical polymerization and gelation. The resulted hydrogel shows directional conductive and mechanical properties, mimicking an oriented biological tissue. Under external electrical stimulation, the orientated PFeCNT nanohybrids can be sensed by the myoblasts cultured on the hydrogel, resulting in the oriented growth of cells. In summary, the mussel-inspired anisotropic hydrogel with its aligned structural complexity and anisotropic properties together with the cell affinity and tissue adhesiveness is a potent multifunctional biomaterial for mimicking oriented tissues to guide cell proliferation and tissue regeneration.

Thermally conductive and electrically insulating polymer/boron nitride (BN) nanocomposites are highly attractive for various applications in many thermal management fields. However, so far most of the preparation methods for polymer/BN nanocomposites have usually caused difficulties in the material post processing. Here, an in situ grafting approach is designed to fabricate thermally conductive, electrically insulating and post-melt processable polystyrene (PS)/BN nanosphere (BNNS) nanocomposites by initiating styrene (St) on the surface functionalized BNNSs via reversible addition fragmentation chain transfer polymerization. The nanocomposites exhibit significantly enhanced thermal conductivity. For example, at a St/BN feeding ratio of 5:1, an enhancement ratio of 1375% is achieved in comparison with pure PS. Moreover, the dielectric properties of the nanocomposites show a desirable weak dependence on frequency, and the dielectric loss tangent of the nanocomposites remains at a very low level. More importantly, the nanocomposites can be subjected to multiple melt processing to form different shapes. Our method can become a universal approach to prepare thermally conductive, electrically insulating and melt-processable polymer nanocomposites with diverse monomers and nanofillers.

Silk fabric reinforced epoxy composites (SFRPs) were prepared by simple hot-press and vacuum treatment, to achieve a maximum reinforcement fraction of 70 vol.%-silk. Mechanical behaviour, specifically tensile, flexural, interlaminar shear, impact, dynamic and thermal properties of the SFRPs, were investigated. It was shown that reinforcement by silk fabric can greatly enhance the mechanical performance of SFRPs. In particular, the tensile modulus and breaking energy of 70 vol.%-silk SFRP were 145% and 467% higher than the pristine epoxy resin. Moreover, the flexural modulus, ultimate strength and breaking energy were also markedly increased for SFRPs. The flexural strength increased linearly with increasing silk volume fraction from 30 to 60 vol.% but diminished slightly at 70 vol.%. Additionally, interlaminar shear results showed that the silk and the matrix epoxy resin had better adhesion properties than plain woven flax fibre. Of most significance is that the impact strength reached a maximum of ~71 kJ/m 2 for the 60 vol.%-silk SFRP, which demonstrates the potential of silk reinforcements in impact-resistant composites for applications such as wind turbine blades. Our study may shed light on improving the strength and toughness of engineering composites by incorporating high volume fractions of natural fibres.

Natural cocoons are an important group of natural fibre composites with versatile functionalities. Previous studies have focused on the diversity of cocoon species and different morphological and mechanical features. It was suggested that the cocoon network structure determined the final mechanical properties of the cocoon composite. Nevertheless, the full structure-propertyfunction relationships for the cocoon composite are not understood. By studying two distinct cocoon species with specific functionalities, we prove that the mechanical properties of two cocoons are determined by both network properties and fibre properties. A robust fibre network is the prerequisite, within which the good mechanical properties of the fibres can play a part. The finding will inspire new designs of synthetic composites with desirable and predictable mechanical properties.

Strong and tough epoxy composites are developed using a less-studied fibre reinforcement, that of natural silk. Two common but structurally distinct silks from the domestic B. mori/Bm and the wild A. pernyi/Ap silkworms are selected in fabric forms. We show that the toughening effects on silk-epoxy composites or SFRPs are dependent on the silk species and the volume fraction of silk. Both silks enhance the room-temperature tensile and flexural mechanical properties of the composite, whereas the more resilient Ap silk shows a more pronounced toughening effect and a lower critical reinforcement volume for the brittle-ductile transition. Specifically, our 60 vol.% Ap-SFRP displays a three-fold elevation in tensile and flexural strength, as compared to pure epoxy resin, with an order of magnitude higher breaking energy via a distinct, ductile failure mode. Importantly, the 60 vol.% Ap-SFRP remains ductile with 7% flexural elongation at lower temperatures (−50 °C). Under impact, these SFRPs show significantly improved energy absorption, and the 60 vol.% Ap-SFRP has an impact strength some eight times that of pure epoxy resin. The findings demonstrate both marked toughening and strengthening effects for epoxy composites from natural silk reinforcements, which presents opportunities for mechanically superior and “green” structural composites.