Electroactive polymers (EAPs) refer to a broad range of relatively soft materials that change size and/or shape upon application of an electrical stimulus. Of these, dielectric elastomers (DEs) generated from either chemically- or physically-crosslinked polymer networks afford the highest levels of electroactuation strain, thereby making this class of EAPs the leading technology for artificial-muscle applications. While mechanically prestraining elastic networks remarkably enhances DEs electroactuation, external prestrain protocols severely limit both actuator performance and device implementation due to gradual DE stress relaxation and the presence of a cumbersome load frame. These drawbacks have persisted with surprisingly minimal advances in the actuation of single-component elastomers since the dawn of the “pre-strain era” introduced by Pelrine et al. (Science, 2000). In this work, we present a bottom-up, molecular-based strategy for the design of prestrain-free (freestanding) DEs derived from covalently-crosslinked bottlebrush polymers. This architecture, wherein design factors such as crosslink density, graft density and graft length can all be independently controlled, yields inherently strained polymer networks that can be readily adapted to a variety of chemistries. To validate the use of these molecularly-tunable materials as DEs, we have synthesized a series of bottlebrush silicone elastomers in as-cast shapes. Examination of these materials reveals that they undergo giant electroactuation strains (>300%) at relatively low fields (<10 V/m), thereby outperforming all commercial DEs to date and opening new opportunities in responsive soft-material technologies (e.g., robotics). The molecular design approach to controlling (electro)mechanical developed here is independent of chemistry and permits access to an unprecedented range of actuation properties from elastomeric materials with traditionally modest electroactuation performance (e.g., polydimethylsiloxane, PDMS). Experimental results obtained here compare favorably with theoretical predictions and demonstrate that the unique behavior of these materials is a direct consequence of the molecular architecture.
Dielectric elastomers (DEs) are the leading technology for artificial muscles due to a favorable combination of large stroke, fast response, and high energy density. However, at large actuations, DEs are prone to spontaneous rupture from electromechanical instability. This shortcoming is currently circumvented by chemical or physical bracing, which increases bulk and rigidity of the total actuator assembly and leads to significant cutbacks in device efficiency and utility. Now, we present a molecular design platform for the creation of freestanding actuators that allow for large stroke (>300%) at low applied fields (<10 V μm-1) in unconstrained as cast shapes. This approach is based on bottlebrush architecture, which features inherently strained polymer networks that eliminate electromechanical instability and the need for bracing. Through accurate control of side-chain length and crosslink density, we obtained effective actuation properties on par with commercial actuators with the advantage of lighter weight, lower voltage operation, and ease of fabrication, which open new opportunities in soft-matter robotics. Furthermore, incorporation of dynamic reversible bonds ensures self-healing of rupture actuators.
Access to the requested content is limited to institutions that have purchased or subscribe to SPIE eBooks.
You are receiving this notice because your organization may not have SPIE eBooks access.*
*Shibboleth/Open Athens users─please
sign in
to access your institution's subscriptions.
To obtain this item, you may purchase the complete book in print or electronic format on
SPIE.org.
INSTITUTIONAL Select your institution to access the SPIE Digital Library.
PERSONAL Sign in with your SPIE account to access your personal subscriptions or to use specific features such as save to my library, sign up for alerts, save searches, etc.