Supramolecular Functionalization Strategy for High Performance Secondary Batteries

The performance and durability of next-generation secondary batteries are governed not only by the intrinsic properties of active materials but also by dynamic interfaces among electrodes, electrolytes, and binders. In this presentation, we introduce supramolecular functionalization strategies designed to regulate interfacial reactions, mechanical integrity, and ion transport in high-energy battery systems. First, polydopamine-derived coatings are used as electrolyte-blocking yet Li-ion-permeable layers to suppress parasitic electrolyte decomposition under lean-electrolyte conditions. Combined with Extremely Lean Electrolyte Testing (ELET), this approach enables quantitative evaluation of electrolyte consumption and cycle life. Second, reversible hydrogen-bonding networks are developed as supramolecular binders to accommodate the large volume changes of silicon anodes. A rheological fatigue-analysis method is further introduced to quantify the persistence of self-healing under repeated deformation, establishing fatigue endurance as a practical binder design criterion. Additional supramolecular approaches will also be discussed, including adhesive conductive networks, interfacially compatibilized carbon precursors for silicon–carbon nanocomposites, and phosphate-mediated surface functionalization for stable fast-charging graphite electrodes. These strategies share a common goal: creating adaptive interphases that simultaneously regulate ion transport, stress dissipation, and interfacial stability. Collectively, these studies demonstrate that supramolecular functionalization offers a versatile platform for overcoming coupled electrochemical and mechanical limitations in advanced batteries. By integrating reversible interactions, interfacial selectivity, and dynamic adaptability, this approach provides new design principles for high-performance lithium-ion and beyond-lithium battery systems.