The structure of the electric double layer: Atomistic versus continuum approaches

• Published in: Current opinion in electrochemistry Vol. 33; p. 100953
• Main Authors: Sakong, Sung, Huang, Jun, Eikerling, Michael, Groß, Axel
• Format: Journal Article
• Language: English
• Published: Elsevier B.V 01.06.2022
• Subjects: Ab initio molecular dynamics simulations; Electric double layer; Electrochemical interfaces; Semiclassical method; Electric double layer; Ab initio molecular dynamics simulations; Semiclassical method; Electrochemical interfaces
• ISSN: 2451-9103; 2451-9111
• DOI: 10.1016/j.coelec.2022.100953

This article reviews recent forays in theoretical modeling of the double layer structure at electrode/electrolyte interfaces by current atomistic and continuum approaches. We will briefly discuss progress in both approaches and present a perspective on how to better describe the electric double layer by combining the unique advantages of each method. First-principles atomistic approaches provide the most detailed insights into the electronic and geometric structure of electrode/electrolyte interfaces. However, they are numerically too demanding to allow for a systematic investigation of the electric double layers over a wide range of electrochemical conditions. Yet, they can provide valuable input for continuum approaches that can capture the influence of the electrochemical environment on a larger length and time scale due to their numerical efficiency. However, continuum approaches rely on reliable input parameters. Conversely, continuum methods can provide a preselection of interface structures and conditions to be further studied on the atomistic level.