Self‐Evolving Gradient Alloy Layer Enables Stable Al Foil Anode for High Energy Lithium Batteries

作者：Sihai Bi, Ruopeng Li, Serhii Kuksenko, Penghui Ren, Mei‐Yan Sun, Yaqiang Li, Xiaona Pan, Guangzhao Wang, Jiang Qin, Anmin Liu, Jinqiu Zhang, Maozhong An, Peixia Yang, Yuanpeng Liu · 发表于：Advanced Materials · 年份：2025 · DOI：10.1002/adma.202514988 · 被引用次数：8 · 研究领域：Advancements in Battery Materials、Advanced Battery Materials and Technologies、Fiber-reinforced polymer composites

Abstract Aluminum (Al) foil anodes, alloyed with lithium (Li), offer a theoretical capacity of 993 mAhg −1 and are considered promising candidates for next‐generation high‐energy‐density lithium‐ion batteries (LIBs). However, their practical application is hindered by non‐uniform alloying processes initiated by the native Al 2 O 3 passivation layer, leading to severe structural degradation and electrode pulverization. Here, a self‐evolving gradient alloy strategy is proposed that enables uniform Li alloying through the in situ construction of a lithiophilic zinc (Zn) interfacial layer on commercial Al foil via a scalable electroless plating process. The Zn interlayer initiates a low‐barrier, sequential alloying pathway—from LiZn to LiAl—thereby promoting uniform lithium infusion, suppressing stress accumulation, and stabilizing the solid–electrolyte interphase (SEI). As a result, the Al@Zn anode achieves an ultralong cycling lifespan with a high Coulombic efficiency of 99.92% over 11 800 cycles, and powers full cells delivering an energy density of 452 Wh kg −1 . Comprehensive structural, electrochemical, and theoretical analyses confirm that the Zn‐guided interfacial gradient effectively mitigates mechanical failure and interfacial instability. This work presents a practical and scalable interfacial engineering approach toward stable, high‐performance alloy‐type anodes, paving the way for the next generation of lithium‐ion batteries.