Triboiontronics for High‐Reliability Sensing: Long‐Term Maintenance of Asymmetric Electrical Double Layers

ABSTRACT Triboiontronic devices achieve mechanical‐to‐electrical signal conversion by dynamically regulating ion migration and the electrical double layer (EDL), offering advantages in flexible sensing and bionic perception. Devices featuring direct electrode–hydrogel contact exhibit high charge transfer densities, but the current output of existing devices decays rapidly with the number of cycles. This current output decay hinders high‐reliability sensing applications. Here, an asymmetric Au/PET‐carbon cloth electrode system was constructed. By leveraging the abundant oxygen‐containing functional groups and porous structure on the surface of the carbon cloth to achieve strong adsorption of Li + , a significantly asymmetric EDL structure was formed and sustained over the long term between the upper and lower electrodes. Leveraging the Hofmeister salting‐out effect of Li + , the pore structure and ionic conductivity of the ionic hydrogel were precisely controlled, increasing mobile ions and enhancing the interfacial contact area to synergistically amplify EDL density. Consequently, the device maintained a stable current output (∼60 µA) over 1000 cycles without significant decay. This study allows the expansion of devices based on similar mechanisms from “attenuated energy harvesting” to the field of “highly stable sensing applications,” providing a new theoretical basis and technical pathway for the design of highly reliable, high‐current‐output triboiontronic sensors.