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Magnetorheological (MR) elastomers are a class of stimuli-responsive materials of which the damping and stiffness can be reversibly tailored by applying magnetic fields. However, concerns such as fatigue damage, insufficient MR efficiencies with low loadings of magnetic particles or highly crosslinked elastomers, and lack of reprocessability remain unaddressed for conventional MR elastomers. To this end, a series of self-healing MR elastomers (SHMRE) were prepared based on thermoreversible Diels–Alder covalent crosslinks. The application of magnetic pulses yielded pre-aligned magnetic particles chains within the curing matrix which strongly influenced the SHMRE rheological properties. The resulting composites do not only exhibit a large MR effect but also efficient self-healing properties at room temperature. We found that the particle loading and the field-induced orientation of the aggregates affect the magnitude of the MR response, the mechanical strength and the healing efficiency. In addition, the MR response is also strongly influenced by the temperature. With a temperature increase from room temperature to 70 °C, a change in the MR response from 90% to 462% is observed while the SHMRE retain a solid viscoelastic state at 50 wt% particles loading. Interestingly, the thermoreversible features of the synthesized networks also allow potential reprocessability of SHMRE when heating these systems above the gel transition temperature (89 °C–90 °C). The final low viscous state makes it possible for the magnetic particles to be potentially restructured as chains by applying a magnetic field, which are retained upon cooling when the solid network state is recovered. The proposed SHMRE systems are shown to be a highly efficient and reprocessable solution to substitute classical MR elastomers in a wider context of generalized MR materials. [ABSTRACT FROM AUTHOR]

Humins waste valorization is considered to be an essential pathway to improve the economic viability of many biorefinery processes and further promote their circularity by avoiding waste formation. In this research, the incorporation of humins in a Diels–Alder (DA) polymer network based on furan-maleimide thermoreversible crosslinks was studied. A considerable enhancement of the healing efficiency was observed by just healing for 1 h at 60 °C at the expense of a reduction of the material mechanical properties, while the unfilled material showed no healing under the same conditions. Nevertheless, the thermal healing step favored the irreversible humins polycondensation, thus strengthening the material while keeping the enhanced healing performance. Our hypothesis states a synergistic healing mechanism based on humins flowing throughout the damage, followed by thermal humins crosslinking during the healing trigger, together with DA thermoreversible bonds recombination. A multi-material soft robotic gripper was manufactured out of the proposed material, showing not only improved recovery of the functional performance upon healing but also stiffness-tunable features by means of humins thermal crosslinking. For the first time, both damage healing and zone reinforcement for further damage prevention are achieved in a single intrinsic self-healing system. [ABSTRACT FROM AUTHOR]

[Display omitted] • A glassy thermoset based on thermoreversible Diels-Alder crosslinks has been manufactured using selective laser sintering. • Powder morphology and flow properties are suitable for selective laser sintering applications. • Built parts show great healing performance, correcting partial curing and porosity generated during printing under a thermal posttreatment. • Built parts are reprocessable and recyclable without altering their chemical nature. Selective Laser Sintering (SLS) is a well-known additive manufacturing technique that builds 3D complex structures by sintering powder particles together upon laser irradiation. In the polymer field, thermoset resins are a popular choice for a plethora of applications due to their great mechanical properties and thermochemical stability. However, due to their irreversible crosslinked nature, they are hard to be processed using SLS. Herein, a covalently crosslinked polymer thermoset based on thermally reversible Diels-Alder (DA) bonds has been printed using SLS. The thermoreversible network exhibits a glassy behavior due to its high crosslinked density and glass transition temperature and was successfully milled into a suitable particle size, morphology and flow for SLS applications. At low temperatures, the DA equilibrium shifts towards the formation of the DA crosslinks, while at high temperatures the DA adducts gradually dissociate, allowing flow and reprocessability at temperatures above 131˚C. Furthermore, the printed parts exhibit healing ability when heated above their glass transition temperature, reaching a fracture stress and Young's Modulus of 25.4 MPa and 1416 MPa, respectively. Thus, the dynamic nature of the network extends the build lifetime upon damage and also brings the opportunity of recycling or reprocessing, enhancing circularity compared to classic thermosets. [ABSTRACT FROM AUTHOR]