To achieve both high
structural integrity and excellent ion transport, designing ion gel
polymer electrolytes (IGPEs) composed of an ionic conducting phase
and a mechanical supporting polymer matrix is one of the promising
material strategies for the development of next-generation all-solid-state
energy storage systems. Herein, we prepared an IGPE thin film, in
which an ion-diffusing phase containing ionic liquids and lithium
salts was bicontinuously intertwined with a cross-linked epoxy phase,
using a silicon elastomer-based stamping method, thus producing a
homogeneous IGPE-based thin film with low surface roughness (R
rms = 0.5 nm). Following the optimization of
the IGPE thin film in terms of the concentrations of ionic constituents,
the film thickness, and various process parameters, the IGPE itself
showed a high ionic conductivity of 0.23 mS/cm with a low activation
energy for lithium-ion transport, as well as the high capacitance
of approximately 10 μF/cm2 based on the metal–insulator–metal
configuration. Furthermore, an all-solid-state supercapacitor containing
two IGPE coating-activated carbon electrodes produced using our poly(dimethylsiloxane)
(PDMS) stamping method exhibited high energy and power densities (44
W h/kg at 875 W/kg and 28 kW/kg at 3 W h/kg). It was also found that
this supercapacitor showed a dramatic reduction (more than 50%) of
the current–resistance (IR) drop, which is
an indicator of low interface resistance, while maintaining the initial
electrochemical performance even after severe mechanical deformation
such as bending or rolling. Therefore, all these results support the
fact that our developed PDMS stamping method enables the rendering
of a high-performance ion gel polymer thin-film-based electrolyte
with acceptable stability and mechanical flexibility for all-solid-state
wearable energy storage devices.