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Unearthing the source of Helmholtz capacitance is vital for comprehensively understanding the interfacial arrangement and electrostatic potential distribution profile of electric double layers (EDL). For a comparative examination, this work integrated ab initio and classical molecular dynamics simulations of the electrified Cu(10/electrolyte and graphene/electrolyte interfaces. A hypothesis was advanced that the Helmholtz capacitance is constructed from three parts connected in series: the typical solvent capacita
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