The use of devulcanized tire powder as an effective reinforcement in self-healing styrene-butadiene rubber (SBR) compounds has been investigated for the first time in this work. For this purpose, the evolution of the microstructure of the rubber from end-of-life tires (ELTs) was studied during granulation, grinding and devulcanization through an exhaustive characterization work in order to relate the final microstructure with the mechanical response of the repaired systems. Different morphologies (particle size distribution and specific surface area) obtained by cryogenic and water jet grinding processes, as well as different devulcanization techniques (thermo-mechanical, microwave, and thermo-chemical), were analyzed. The results demonstrated the key influence of the morphology of the ground tire rubber (GTR) on the obtained devulcanized products (dGTR). The predictions of the Horikx curves regarding the selectivity of the applied devulcanization processes were validated, thereby; a model of the microstructure of these materials was defined. This model made it possible to relate the morphology of GTR and dGTR with their activity as reinforcement in self-healing formulations. In this sense, higher specific surface area and percentage of free surface polymeric chains resulted in better mechanical performance and more effective healing. Such a strategy enabled an overall healing efficiency of more than 80% in terms of a real mechanical recovery (tensile strength and elongation at break), when adding 30 phr of dGTR. These results open a great opportunity to find the desired balance between the mechanical properties before and after self-repair, thus providing a high technological valorization to waste tires.

In the present work, the effectiveness of four non-halogenated flame retardants (FR) (aluminium trihydroxide (ATH), magnesium hydroxide (MDH), Sepiolite (SEP) and a mix of metallic oxides and hydroxides (PAVAL)) in blends with recycled acrylonitrile-butadiene-styrene (rABS) was studied in order to develop a more environmentally friendly flame-retardant composite alternative. The mechanical and thermo-mechanical properties of the obtained composites as well as their flame-retardant mechanism were evaluated by UL-94 and cone calorimetric tests. As expected, these particles modified the mechanical performance of the rABS, increasing its stiffness at the expense of reducing its toughness and impact behavior. Regarding the fire behavior, the experimentation showed that there is an important synergy between the chemical mechanism provided by MDH (decomposition into oxides and water) and the physical mechanism provided by SEP (oxygen barrier), which means that mixed composites (rABS/MDH/SEP) can be obtained with a flame behavior superior to that of the composites studied with only one type of FR. In order to find a balance between mechanical properties, composites with different amounts of SEP and MDH were evaluated. The results showed that composites with the composition rABS/MDH/SEP: 70/15/15 wt.% increase the time to ignition (TTI) by 75% and the resulting mass after ignition by more than 600%. Furthermore, they decrease the heat release rate (HRR) by 62.9%, the total smoke production (TSP) by 19.04% and the total heat release rate (THHR) by 13.77% compared to unadditivated rABS; without compromising the mechanical behavior of the original material. These results are promising and potentially represent a greener alternative for the manufacture of flame-retardant composites.