Battery-supercapacitor hybrid devices (BSHDs) are meant to fulfil the gap existing between conventional batteries and traditional supercapacitors by exhibiting high-energy and high-power densities, added to excellent cycling stabilities. Nonetheless, effectively integrating the diverse energy storage mechanisms of batteries and supercapacitors remains a significant challenge. Various approaches have been proposed to mitigate these issues ranging from developing advanced microstructures to engineering the interface between electrode|current collector or electrode|electrolyte.1 Previously, our team documented the fabrication of BSHDs capable of undergoing 3,000 charge-discharge cycles while maintaining 81% of their initial capacity.2 This work presents an upgraded iteration of BSHDs which maintains over 95% of the initial capacity and notably increasing the lifespan to over 10,000 cycles. The device in question is composed by a protected graphite anode and a solid electrolyte, composed by either an alginate polymer network or commercially available glass microfiber, with an ionic liquid (PP13-FSI; 1-Methyl-1-propylpyrrolidinium Bis(fluorosulfonyl)imide) as the ion conductive electrolyte. The improvement was achieved by conducting a thorough analysis and optimization of the solid electrolyte in response to the device’s performance during lithium-intercalation, i.e. introducing charge to the anode by forming a stable solid-electrolyte interface (SEI), added to the capability of such said anode as counter electrode during the operation of an activated carbon capacitor.This work therefore discusses the duality between the maximum capacity obtained during the SEI formation process vs the capacity and anode potential retention during the operation of the BSHD, deep diving into the relationship of, inter alia, the thickness of the SEI formed, the increase or decrease of the ion-desolvation resistances, ionic conductivities, and activation energies versus the overall performance of the device.
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