Dynamic Contributions to the Bulk Mechanical Properties of Self-Assembled Polymer Networks with Reconfigurable Bonds.

Soft materials that contain dynamic and reversible bonds exhibit unique properties including unusual extensibility, reversible elasticity, and self-healing capabilities, for example. Catechol motifs are of particular interest owing to their ability to form many kinds of reversible bonds; however, there are few reports on the role of hydrogen bonds between catechols. Here, physically crosslinked self-assembled networks composed of catechol-functionalized ABA triblock co-polymers are synthesized and characterized to elucidate the role of intermolecular bonding between catechol motifs on bulk mechanical properties. The Young's moduli of equilibrated networks range from 16 to 43 MPa. Furthermore, the concentration of intermolecular interaction is controlled indirectly by synthesizing polymers with prescribed catechol concentrations on each A block. Further, network dynamics are characterized by measuring the relaxation spectrum, and it is found that the network mean relaxation time is inversely related to catechol density. Finally, networks exhibit time-dependent recovery after uniaxial strain. These findings establish important relationships between molecular design, network composition, and macroscopic mechanical properties of model soft matter networks with dynamic intermolecular bonds. Furthermore, this insight has the potential to guide the design of dissipative materials for use in applications ranging from consumer products to surgical materials.

Characterization of Temperature and Humidity Dependence in Soft Elastomer Behavior.

Soft robots are predicted to operate well in unstructured environments due to their resilience to impacts, embodied intelligence, and potential ability to adapt to uncertain circumstances. Soft robots are of further interest for space and extraterrestrial missions, owing to their lightweight and compressible construction. Most soft robots in the literature to-date are made of elastomer bodies. However, limited data are available on the material characteristics of commonly used elastomers in extreme environments. In this study, we characterize four commonly used elastomers in the soft robotics literature-EcoFlex 00-30, Dragon Skin 10, Smooth-Sil 950, and Sylgard 184-in a temperature range of -40°C to 80°C and humidity range of 5-95% RH. We perform pull-to-failure, stiffness, and stress-relaxation tests. Furthermore, we perform a case study on soft elastomers used in stretchable capacitive sensors to evaluate the implications of the constituent material behavior on component performance. We find that all elastomers show temperature-dependent behavior, with typical stiffening of the material and a lower strain at failure with increasing temperature. The stress-relaxation response to temperature depends on the type of elastomer. Limited material effects are observed in response to different humidity conditions. The mechanical properties of the capacitive sensors are only dependent on temperature, but the measured capacitance shows changes related to both humidity and temperature changes, indicating that component-specific properties need to be considered in tandem with the mechanical design. This study provides essential insights into elastomer behavior for the design and successful operation of soft robots in varied environmental conditions.

Soft Actuators Made of Discrete Grains.

Recent work has demonstrated the potential of actuators consisting of bulk elastomers with phase-changing inclusions for generating high forces and large volumetric expansions. Simultaneously, granular assemblies have been shown to enable tunable properties via different packings, dynamic moduli via jamming, and compatibility with various printing methods via suspension in carrier fluids. Herein, granular actuators are introduced, which represent a new class of soft actuators made of discrete grains. The soft grains consist of a hyperelastic shell and multiple solvent cores. Upon heating, the encapsulated solvent cores undergo liquid-to-gas phase change, inducing rapid and strong volumetric expansion of the hyperelastic shell up to 700%. The grains can be used independently for micro-actuation, or in granular agglomerates for meso- and macroscale actuation, demonstrating the scalability of the granular actuators. Furthermore, the active grains can be suspended in a carrier resin or solvent to enable printable soft actuators via established granular material processing techniques. By combining the advantages of phase-change soft actuation and granularity, this work presents the opportunity to realize soft actuators with tunable bulk properties, compatibility with self-assembly techniques, and on-demand reconfigurability.