A Highly Conductive, Stretchable, and Healable Sensing Electrode Consisting of PEDOT Conductive Pathway and Semi‐Interpenetrating Network

Abstract Flexible dry electrode provides an ideal material for the application of wearable electronic devices. The conductive polymer PEDOT:PSS has received wide attention for its adjustable electrical, mechanical, and adhesion properties. However, it remains a challenges to systematically optimize performances as the restriction between insulating PSS chains and rigid PEDOT backbone. In this paper, a highly conductive, stretchable, and healable electrode is designed by blending poly(ethylene dioxythiophene): poly(styrene sulfonate) (PEDOT:PSS) with polyvinylpyrrolidone (PVP), polyvinyl alcohol (PVA), and tannic acid (TA). The blended film exhibits a two‐phase separation structure. The backbone in PEDOT‐phase forms conformational transformation and aggregation to construct conductive pathways. PVP and poly (styrene sulfonate) (PSS) chains percolate into the PVA/TA crosslinked network through hydrogen bonds, forming a PVA/PVP/PSS semi‐interpenetrating network. The PEDOT:PSS/PVA/PVP/TA film exhibits excellent electrical (1300 S cm −1 ) and mechanical (266% strain) properties, the resistance can remain stable (R/R 0 = 1.06) after 3000 cycles of stretching at 100% strain. Furthermore, the water‐induced approach is chosen to heal the damaged film, the conductivity will be fully restored, and tensile properties are restored to 48%. The wearable electrode can efficiently acquire electromyography (EMG) and electrocardiography (ECG) signals, and conduct monitoring of different respiratory states. Healable film offers the prospect of more applications and longer service life for electronic products.