Ionic Rectification by Dynamic Regulation of the Electric Double Layer at the Hydrogel Interface

Hydrogels play a pivotal role in the realm of iontronics, contributing to the realization of futuristic human–machine interactions. The electric double layer (EDL) between the hydrogel and electrode provides an essential ionic–electronic coupling interface. While prior investigations primarily delved into elucidating the formation mechanism of the EDL, our study shifts the focus to showcasing the current generation through the mechanical modulation of the EDL at the hydrogel–metal interfaces. The dynamic EDL was constructed by the mechano-driven contact–separation process between the polyacrylamide (PAAm) hydrogel and Au. Influencing factors on the dynamic regulation of the EDL such as ion concentration, types of salt, contact–separation frequency, and deformation degree were investigated. Dehydration usually limits the practical applications of hydrogels, and it is a long-standing and difficult problem. However, it seemed to be able to slow the EDL formation process here, resulting in a sustained continuous direct current signal output. Such hydrogel iontronics could rectify the displacement electronic current of a triboelectric nanogenerator by the ionic current. The directional migration of ions could be further enhanced by using charge-collecting metals with different work functions, for example, Au and Al. It offers a paradigm to enable ionic rectification that could be seamlessly incorporated into electronic systems, ushering in a new era for efficient energy harvesting and biomimetic nervous systems.