Cation–π Interactions in Graphene‐Containing Systems for Water Treatment and Beyond

Abstract Cation–π interactions are common in nature, especially in organisms. Their profound influences in chemistry, physics, and biology have been continuously investigated since they were discovered in 1981. However, the importance of cation–π interactions in materials science, regarding carbonaceous nanomaterials, has just been realized. The interplay between cations and delocalized polarizable π electrons of graphene would bring about significant changes to the intrinsic characteristics of graphene and greatly affect the device performance based on graphene and its derivatives. Here, the cation–π interactions in graphene containing systems for water treatment applications (e.g., separation membranes, adsorbents) are highlighted. The cross‐linking effects caused by cation–π interactions contribute to membrane stability and selectivity and enhanced adsorption. Their roles in dominating the performance of graphene‐based structures for other specific applications are also discussed. Relevant theoretical modeling and calculations are summarized to offer an in‐depth understanding of the underlying mechanisms which can help in designing more functional materials and structures. Perspectives on the potential directions that deserve effort are also presented.