Shape-memory polymers tend to present rigid behavior at ambient temperature, being unable to deform in this state. To obtain soft shape-memory elastomers, composites based on a commercial rubber crosslinked by both ionic and covalent bonds were developed, as these materials do not lose their elastomeric behavior below their transition (or activation) temperature (using ionic transition for such a purpose). The introduction of fillers, such as carbon black and multiwalled carbon nanotubes (MWCNTs), was studied and compared with the unfilled matrix. By adding contents above 10 phr of MWCNT, shape-memory properties were enhanced by 10%, achieving fixing and recovery ratios above 90% and a faster response. Moreover, by adding these fillers, the conductivity of the materials increased from ~10−11 to ~10−4 S·cm−1, allowing the possibility to activate the shape-memory effect with an electric current, based on the heating of the material by the Joule effect, achieving a fast and clean stimulus requiring only a current source of 50 V.

There are currently many well-established applications for recycled rubber from end-of-life tires (ELT), but it is essential to investigate and seek new approaches to enhance the value of these products. Recent developments in new technologies and innovative recycling and devulcanization processes have opened up new perspectives for ELT crumb rubber. To promote the use of these products in newly added value applications, it is essential to develop and optimize methods that allow the characterization of parameters related to the ultimate properties of potential final applications. In this respect, a novel characterization methodology based on advanced 1H double-quantum (DQ) nuclear magnetic resonance experiments has been applied for the first time to quantify the key parameters that characterize the structure of ELT crumb rubber after diverse recycling processes: from simple mechanical grinding to complex devulcanization methods. This experimental approach enables the quantification of parameters that define the network structure of rubber, such as the nonelastic network defects (sol fraction, dangling chain ends, loops), the cross-link density, and the heterogeneity of the network, directly from rubber granulate and powder (without any additional sample preparation steps), overcoming most of the drawbacks and uncertainties that limit the application of traditional rubber characterization methods (e.g., equilibrium swelling experiments). By applying this experimental approach, it is possible to identify and quantify the actual technical limits for a complete selective devulcanization process of ELT crumb rubber.

Many efforts are being made to find innovative ways of recycling rubber from end-of-life tires (ELTs), also called ground tire Rubber (GTR). Recycling through devulcanization allows the reintroduction of rubber back into the manufacturing industry. Such a process requires providing enough energy to break the sulfur links, while preventing damage to the polymeric chain. Microwave heating is controllable, efficient, and it does not rely on conventional heating mechanisms (conduction, convection) which may involve high heating losses, but rather on direct dielectric heating. However, to adequately control the microwave-assisted devulcanization performance, a thorough knowledge of the GTR permittivity versus temperature is required. In this work, GTR permittivity was monitored during its devulcanization. A resonant technique based on a dual-mode cylindrical cavity was used to simultaneously heat rubber and measure its permittivity at around 2 GHz. The results show sharp changes in the GTR permittivity at 160 and 190 °C. After the GTR cooled down, a shifted permittivity evidences a change in the GTR structure caused by the devulcanization process. Microwave-assisted devulcanization effectiveness is proven through time-domain nuclear magnetic resonance (NMR) measurements, by verifying the decrease in the cross-link density of processed GTR samples compared to the original sample.