Ionic liquids (ILs) have emerged as a novel class of chemical compounds for the development of advanced (multi)functional materials with outstanding potential in applications of several areas due to their unique properties and functionalities. The combination of ILs with polymers, in a composite, allows for developing smart materials, which synergistically combine the features of specific polymers and ILs. Moreover, ILs can be extensively modified by the incorporation of functional groups with specific properties into the cation, anion, or both. Thus, it is possible to tune the IL, the polymer, or both to obtain a broad spectrum of multifunctional composites and address the specific requirements of many applications. This work focusses on advanced materials and strategies concerning ILs and polymers for the development of smart IL/polymer‐based materials for applications including responsive and sensitive sensors, actuators, environment, batteries, fuel cells, and biomedical applications.

Protein-based polymers are present in a wide variety of organisms fulfilling structural and mechanical roles. Advances in protein engineering and recombinant DNA technology allow the design and production of recombinant protein-based polymers (rPBPs) with an absolute control of its composition. Although the application of recombinant proteins as biomaterials is still an emerging technology, the possibilities are limitless and far superior to natural or synthetic materials, as the complexity of the structural design can be fully customized. In this work, we report the electrospinning of two new genetically engineered silk-elastin-like proteins (SELPs) consisting of alternate silk- and elastin-like blocks. Electrospinning was performed with formic acid and aqueous solutions at different concentrations without addition of further agents. The size and morphology of the electrospun structures was characterized by scanning electron microscopy showing its dependence on the concentration and solvent used. Treatment with methanol-saturated air was employed to stabilize the structure and promote water insolubility through a time-dependent conversion of random coils into β-sheets (FTIR). The resultant methanol-treated electrospun mats were characterized for swelling degree (570-720%), water vapour transmission rate (1083 g/m(2)/day) and mechanical properties (modulus of elasticity ∼126 MPa). Furthermore, the methanol-treated SELP fibre mats showed no cytotoxicity and were able to support adhesion and proliferation of normal human skin fibroblasts. Adhesion was characterized by a filopodia-mediated mechanism. These results demonstrate that SELP fibre mats can provide promising solutions for the development of novel biomaterials suitable for tissue engineering applications.

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β-Poly(vinylidene fluoride) (β-PVDF) exhibits ferroelectric properties due to the special arrangement of the chain units in the crystalline phase. The piezoelectric properties of the material can be optimised by poling the original stretched film. The main effect of the poling process is the alignment of the randomly organised dipolar moments against the applied field. In this work, poled and non-poled β-PVDF from the same batch are characterised by dielectric spectroscopy. The origin of the electrical and mechanical response of poled and non-poled β-PVDF were further explored by far IR spectroscopy and discussed on a molecular level. The main effect of the poling process on the dielectric response of the material is a small increase of the dielectric constant due to the preferential alignment of the main dipolar contribution and a slight decrease of the dielectric loss, due to the more organized amorphous structure. The conductivity is strongly increased by poling, especially the high-temperature conductivity, ascribed mainly to hopping conductivity due to free charges induced during poling. FTIR experiments indicate that the origin of these effects and also of the variations in the thermo-mechanical response of the material can be found in the reorientation of the crystalline dipoles along the poling field, together with a partial reduction of the amount of α phase and an increase of the amount of β phase. The α to β transformation, mainly due to the stretching process, seems to be optimized by the poling process.

Environmental issues promote the development of sensors based on natural polymers which are becoming an area of increasing interest.

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