Harder dielectric elastomers are structurally stronger than soft ones but hardly actuate under electrostatic pressure. It remains unclear which property limits harder dielectric elastomers from producing as large actuation as soft ones. This study shows that the change in stretch limit rather than modulus bounds the ultimate dielectric actuation. A larger ultimate stretch warrants a pre-stretched membrane to further thin down and expand biaxially relative to the pre-stretch state. Theory and experiments showed that pre-stretch alters the maximum stretchability and ultimate dielectric actuation. An optimal pre-stretch helps maximize the ultimate actuation close to times radially so long as the corresponding total stretch did not exceed the elastomer’s fracture limit. Hence, a stretchy harder dielectric elastomer stands a chance of producing as large ultimate actuation as soft ones do. To validate the theory, we tested three commercial grades of styrene–ethylene/butylene–styrene copolymers (SEBS) organogels with different oil content and shore hardness. The tests showed that a 20 A-hardness organogel of low toughness actuated less ultimately, but a 10 A-hardness organogel of greater toughness actuated as much as an 8 A-hardness organogel does. This 10 A-hardness SEBS organogel showed an ultimate elongation of 1192%, and 3.1 times the shear modulus and seven times the tensile strength of 3 M VHB 4910. When being optimally pre-stretched for 3.5 times radially, it produced a substantial hyperelastic dielectric actuation up to 104% active areal strain at 277 MV m−1, comparable to the actuation generated by the over-stiffened VHB DEAs. Unlike VHB DEAs, these harder SEBS DEAs generated hyperelastic actuation free from severe viscoelastic drift. The high performance of SEBS organogels can potentially meet the need for forceful artificial muscles to drive bio-inspired robots.
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