Collectively Exhaustive Electrodes Based on Covalent Organic Framework and Antagonistic Co‐Doping for Electroactive Ionic Artificial Muscles

Abstract In this study, high‐performance ionic soft actuators are developed for the first time using collectively exhaustive boron and sulfur co‐doped porous carbon electrodes (BS‐COF‐Cs), derived from thiophene‐based boronate‐linked covalent organic framework (T‐COF) as a template. The one‐electron deficiency of boron compared to carbon leads to the generation of hole charge carriers, while sulfur, owing to its high electron density, creates electron carriers in BS‐COF‐C electrodes. This antagonistic functionality of BS‐COF‐C electrodes assists the charge‐transfer rate, leading to fast charge separation in the developed ionic soft actuator under alternating current input signals. Furthermore, the hierarchical porosity, high surface area, and synergistic effect of co‐doping of the BS‐COF‐Cs play crucial roles in offering effective interaction of BS‐COF‐Cs with poly(3,4‐ethylenedioxythiophene) polystyrene sulfonate (PEDOT:PSS), leading to the generation of high electro‐chemo‐mechanical performance of the corresponding composite electrodes. Finally, the developed ionic soft actuator based on the BS‐COF‐C electrode exhibits large bending strain (0.62%), excellent durability (90% retention for 6 hours under operation), and 2.7 times higher bending displacement than PEDOT:PSS under extremely low harmonic input of 0.5 V. This study reveals that the antagonistic functionality of heteroatom co‐doped electrodes plays a crucial role in accelerating the actuation performance of ionic artificial muscles.