Roll‐To‐Roll Production of Li‐Rich Binary Alloy Anodes for Durable, High‐Rate Lithium–Metal Batteries

Abstract Lithium (Li) metal batteries (LMBs) are among the most promising next‐generation energy storage systems, but their practical deployment is hindered by severe dendrite growth. The key challenges for achieving long cycle life and high‐rate capability are the scarcity of lithiophilic sites and sluggish ionic diffusion at the anode surface. Here, a roll‐to‐roll metallurgical strategy is reported in which Li 9 Al 4 (LA) inhibits the growth of Li 22 Sn 5 (LS) within Li metal. Controlled rolling and reduced interfacial energy create favorable thermodynamic and kinetic conditions, enabling trace LA and LS to be homogeneously distributed throughout the anode. This architecture provides abundant lithiophilic sites and appropriate diffusion barriers, ensuring uniform plating/stripping and suppressing dendrite formation. Therefore, symmetric cells exhibit stable cycling with low overpotential for more than 5500 h, and the assembled full cells retain 98.42% of their capacity after 1000 cycles at 5 C. This continuous metallurgical approach offers a scalable pathway toward durable, high‐rate LMBs and represents a paradigm shift for Li metal anode design.