Self‐Evolving Gradient Alloy Layer Enables Stable Al Foil Anode for High Energy Lithium Batteries
Abstract
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.
Article Details
Authors (14)
Sihai Bi
MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage School of Chemistry and Chemical Engineering Harbin Institute of Technology Harbin Heilongjiang 150001 P. R. China
Ruopeng Li
MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage School of Chemistry and Chemical Engineering Harbin Institute of Technology Harbin Heilongjiang 150001 P. R. China
Serhii Kuksenko
MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage School of Chemistry and Chemical Engineering Harbin Institute of Technology Harbin Heilongjiang 150001 P. R. China
Penghui Ren
Zhejiang Key Laboratory of Quantum State Control and Optical Field Manipulation, Department of Physics, Zhejiang Sci-Tech University 1 , Hangzhou 310018,
Meiyan Sun
Department of Anesthesiology and Perioperative Medicine, The Second Affiliated Hospital of Anhui Medical University, Hefei, China (M.S., S.H., Y.Z.).
Yaqiang Li
Institute of Molecular Engineering Plus, College of Chemistry
Xiaona Pan
School of Chemistry and Chemical Engineering State Key Laboratory of Crystal Materials Shandong University Jinan 250100 P. R. China
Guangzhao Wang
Key Laboratory of Extraordinary Bond Engineering and Advanced Materials Technology of Chongqing, School of Electronic Information Engineering, Yangtze Normal University 2 , Chongqing 408100,
Jiang Qin
School of Energy Science and Engineering, Harbin Institute of Technology Harbin 150001 P. R. China
Anmin Liu
Jinqiu Zhang
School of Physical Science and Technology, Ningbo University 1 , Ningbo 315211,
Maozhong An
MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage School of Chemistry and Chemical Engineering Harbin Institute of Technology Harbin Heilongjiang 150001 P. R. China
Peixia Yang
MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage School of Chemistry and Chemical Engineering Harbin Institute of Technology Harbin Heilongjiang 150001 P. R. China
Yuanpeng Liu