Atomistic molecular dynamics simulations were used to investigate the processes of electrical double layer formation and electrolyte confinement in graphene-based supercapacitors. For both processes, free energy calculations were used to analyze the thermodynamics involved in the electrolyte confinement and its re-arrangement in a double layer on the electrode surface. The value of the free energy of the formation of the double electric layer was related to the energy required to charge the supercapacitor, i.e., the energy density stored, and compared with values obtained using Poisson’s electrostatic formalism, which is the conventionally employed approach. Both analyzes were consistent with each other, presenting compatible values for the stored energy.

中文翻译：

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从电学和热力学的角度来看，双电层的形成和在石墨烯基超级电容器上的储能过程。

原子分子动力学模拟用于研究石墨烯基超级电容器中电双层形成和电解质限制的过程。对于这两个过程，使用自由能计算来分析涉及电解质限制及其在电极表面双层中的重新排列的热力学。形成双电层的自由能的值与给超级电容器充电所需的能量有关，即所存储的能量密度，并与使用泊松的静电形式学获得的值进行比较，这是常规采用的方法。两种分析彼此一致，给出了存储能量的兼容值。