Conjugated System of PEDOT:PSS-Induced Self-Doped PANI for Flexible Zinc-Ion Batteries with Enhanced Capacity and Cyclability

Owing to its electronic conductivity and electrochemical reactivity, polyaniline (PANI) can serve as the cathode for rechargeable zinc-ion batteries (ZIBs). However, it suffers from fast deactivation and thus performance deterioration because of spontaneous deprotonation during charge/discharge. Here, we report an effective strategy to improve the electrochemical reactivity and stability of the PANI-based cathode by constructing a π-electron conjugated system between PANI and poly(3,4-ethylenedioxythiophene) polystyrene sulfonate (PEDOT:PSS) on carbon nanotubes (CNTs). The impressive performance of the post-treated CNTs–PANI–PEDOT:PSS (t-CNTs–PA–PE) cathode is largely attributed to the −SO3–H+ groups in PSS, which acts as an internal proton reservoir and provides enough H+ for PANI’s protonation, thus promoting its electrochemical activity and reversibility. Besides, the strong interactions between PANI and PEDOT:PSS assist the stretching of π–π conjugation chains, bringing about enhanced electronic conductivity. Consequently, the t-CNTs–PA–PE cathode achieves a high capacity of 238 mA h g–1, together with good rate capability and long-term stability (over 1500 cycles with 100% Coulombic efficiency). Through exerting the freestanding t-CNTs–PA–PE, a flexible ZIB was further constructed with both outstanding electrochemical properties and superior high safety. This work demonstrates the availability of conducting polymer cathodes for high-performance ZIBs, fulfilling the need of flexible electronics.