Ionic electroactive polymer (iEAP) actuators are recognized as exceptional candidates for artificial muscle development, with significant potential applications in bionic robotics, space exploration, and biomedical fields. Here, we developed a new iEAP actuator utilizing high-purity single-walled carbon nanotubes (SWCNTs)-reinforced poly(3, 4-ethylenedioxythiophene)/poly(4-styrenesulfonate) (PEDOT: PSS, PP) hybrid electrodes and a Nafion/EMIBF4 ion-exchange membrane via a straightforward and efficient spray printing technique. The SWCNT/PP actuator exhibits significantly enhanced electric conductivity (262.9 S/cm) and specific capacitance (22.5 mF/cm2), benefitting from the synergistic effect between SWCNTs and PP. These improvements far surpass those observed in activated carbon aerogel bucky-gel-electrode-based actuators. Furthermore, we evaluated the electroactive behaviors of the SWCNT/PP actuator under alternating square-wave voltages (1–3 V) and frequencies (0.01–100 Hz). The results reveal a substantial bending displacement of 6.44 mm and a high bending strain of 0.61% (at 3 V, 0.1 Hz), along with a long operating stability of up to 10,000 cycles (at 2 V, 1 Hz). This study introduces a straightforward and efficient spray printing technique for the successful preparation of iEAP actuators with superior electrochemical and electromechanical properties as intended, which hold promise as artificial muscles in the field of bionic robotics.
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