Prospect for Supramolecular Chemistry in High-Energy-Density Rechargeable Batteries

Three high-energy-density electrode materials, namely silicon (Si) anodes, lithium (Li) metal anodes, and sulfur cathodes operating by alloying, electroplating, and electrochemical conversion, respectively, have gained discernable interest owing to their unparalleled theoretical capacity. Nevertheless, these electrode materials entail new intrinsic drawbacks, such as massive volume change for Si, uncontrollable lithium dendritic growth for Li metal, and the formation of soluble lithium polysulfides as well as their shuttling for sulfur cathodes. In this Perspective, we discuss how supramolecular chemistry and/or mechanically interlocked molecules and polymers, such as rotaxanes or entangled polymer networks, can play a pivotal role in addressing these challenges facing rechargeable batteries. We introduce the concepts of supramolecular chemistry and their working principles in high-energy-density electrode materials in Li-ion batteries.