Abstract
Summary The description of electrode–electrolyte interfaces is based on the notion of the formation of an electric double layer (EDL). Most of the concepts underlying its structure and properties have been developed more than one hundred years ago based on continuum approaches. Still, a complete atomistic theoretical description is missing. Here, first the traditional models of the EDL will be briefly reviewed before recent atomistic first-principles approaches using either explicit aqueous electrolytes or a grand-canonical formalism will be presented. Finally, the importance of the formation of an EDL at electrode/electrolyte interfaces in batteries will be discussed.
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