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Graphene-based supercapacitors have gained significant attention due to their exceptional energy storage capabilities. Despite numerous research efforts trying to improve the performance, the challenge of experimentally elucidating the nanoscale-interface molecular characteristics still needs to be tackled for device optimizations in commercial applications. To address this, we have conducted a series of experiments using substrate-free graphene field-effect transistors (SF-GFETs) and oxide-supported graphene field-effect transistors (OS-GFETs) to elucidate the graphene-electrolyte interfacial arrangement and corresponding capacitance under different surface potential states and ionic concentration environments.

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