Tailoring Adsorption Properties of Graphitic Surfaces: Toward Improved Anode Materials for Li‐ and Post‐Li Ion Batteries

The adsorption of alkali metal (AM) atoms on graphitic surfaces is one of the processes that determine the performance of carbon‐based anode materials. In particular, when graphite derivatives such as hard carbon with increased surface area are considered, adsorption accounts for a significant amount of the AM storage capacity. While it is well known that the adsorption of Li and Na on pristine graphite is energetically unfavorable, this article shows how graphitic surfaces can be modified to tailor their adsorption properties. For this purpose, the adsorption of Li, Na, and K on graphitic model systems, containing defects and impurities as well as combinations thereof, is investigated by means of density functional theory. The results show that particular defects and impurity atoms can modify the adsorption strength of the surface such that Li and Na adsorption become energetically favorable, while at the same time, capacity loss via trapping of AM atoms is minimized.