Tailoring ion dynamics in energy storage conductors for ultra-stable, high-performance solid-state microsupercapacitor array

All-solid-state electrochemical energy storage (EES) devices with prolonged lifetime, operational stability, and mechanical flexibility can be a promising route to powering up wearable electronics. However, conventional EES devices have been often hindered by a gradual decrease in energy capacity due to low ionic conducting electrolytes, non-suitable electrode materials, or poor electrode/electrolyte interfaces. Herein, we propose a harmonization of the molecular-level tailoring of ionic gel polymer electrolyte (IGPE) and graphene-based electrodes, significantly improving and sustaining the electrochemical performance (11.9 μWh cm⁻²) of EES microsupercapacitor (MSC) devices. Our optimized MSC device based on ethyl-3-methylimidazolium bis(fluorosulfonyl)imide (EMIM-FSI) and interdigitated reduced-graphene oxide (rGO) electrode array maintains 99 % of the initial electrochemical capacity even after 20,000 cycles, also demonstrating the excellent mechanical flexibility (bending radius up to 4 mm) and environmental stability (>30 days) of the MSC-based array. Molecular-level simulation and spectroscopic atomic analysis revealed noticeably lower residual ionic liquid (IL) molecules of EMIM-FSI, compared to EMIM-trifluoromethyl FSI, between the graphene-based layers of electrodes during the charge/discharge cycles. Therefore, our optimization strategy and findings will pave the way to accomplish next-generation of all-solid-state EES devices with ultra-high operational stability, powering wearable electronics.