Crucial interactions of functional pyrenes with graphite in electrodes for lithium‐ion batteries

Polycyclic aromatic hydrocarbons, such as pyrenes, are a well‐known material class for non‐covalent modification of carbon surfaces in many applications. In electrochemical energy storage, pyrenes are mostly used in large polymeric structures. This work addresses the use of carboxy‐ and amino‐functionalized pyrenes for graphite electrodes for lithium‐ion batteries (LIBs). Pyrenes are explored as adsorbed species on graphite prior to electrode fabrication and as additives to the electrode composition. Thereby, 1‐pyrenecarboxylic acid, 1‐pyrenebutyric acid, 1‐aminopyrene, and 1‐pyrenebutylamine were under investigation. As additives, pyrenes do not influence the cycling performance of the electrode at low current but deteriorate the performance at high current, regardless of the functional group. However, when the pyrenes are adsorbed to the graphite surface, the influence of the different functional groups becomes clearly visible, revealing that an additional butyl group has a positive impact on the cycling performance and lithium‐ion transport of the electrodes. Electrodes with 1‐pyrenebutyric acid even enhanced the performance compared to the pristine electrode. Functional pyrenes were used to study the influence of carboxy and amino groups on the electrochemical performance of graphite electrodes in lithium‐ion batteries (LIBs). Remarkable differences in capacities depending on the functional groups are observed when the pyrenes are adsorbed to the graphite surface. To emphasize the importance of the surface modification, the pyrenes were also investigated as additives in graphite electrodes.