Body-temperature programmable elastic shape memory hybrids (SMHs) have great potential for the comfortable fitting of wearable devices. Traditionally, shore hardness is commonly used in the characterization of elastic materials. In this paper, the evolution of shore hardness in body-temperature programmable elastic SMHs upon cyclic loading, and during the shape memory cycle, is systematically investigated. Upon cyclic loading, similar to the Mullins effect, significant softening appears, when the applied strain is over a certain value. On the other hand, after programming, in general, the measured hardness increases with increase in programming strain. However, for certain surfaces, the hardness decreases slightly and then increases rapidly. The underlying mechanism for this phenomenon is explained by the formation of micro-gaps between the inclusion and the matrix after programming. After heating, to melt the inclusions, all samples (both cyclically loaded and programmed) largely recover their original hardness.
12 September 2026 in Advanced Functional Materials
Direct ink writing (DIW) using frontal ring‐opening metathesis polymerization (FROMP) enables rapid, energy‐efficient fabrication of thermoset and elastomeric architectures through a self‐propagating exothermic curing reaction. However, FP‐DIW is constrained by stringent rheological requirements, feature‐size limits from front quenching, and the need for the reaction front to track the nozzle. Here, we overcome these constraints by leveraging embedded 3D printing to implement FP‐DIW with delayed solidification, thereby decoupling shape retention and solidification from ink chemistry and rheology. A yield‐stress support medium stabilizes low‐viscosity inks, suppresses gravitational and capillary instabilities, mitigates quenching at small diameters, and enables complex overlapping and mechanically interlinked features to fuse after deposition. Two thermal initiation strategies are introduced: volumetric dielectric heating via microwaves and surface heating at the support‐bath boundary. Dicyclopentadiene (DCPD), cyclooctadiene (COD), and mixed formulations provide tunable mechanical properties with glass transition temperatures from –50°C to 160°C. The approach enables lattices, springs, mechanically interlocked structures, and multimaterial architectures, substantially expanding the accessible material, feature‐size, and geometric design space compared with FP‐DIW in air.