Decoding Interfacial Evolution of Aluminum Anode and Constructing Multifunctional Layers toward Ultra-Long Cycle Stability

TY - JOUR

T1 - Decoding Interfacial Evolution of Aluminum Anode and Constructing Multifunctional Layers toward Ultra-Long Cycle Stability

AU - Long, Bo

AU - Wu, Feng

AU - Li, Yu

AU - Wang, Huaizhi

AU - Liu, Wenhao

AU - Li, Ying

AU - Li, Qiaojun

AU - Zhou, Qiannan

AU - Bai, Ying

AU - Wu, Chuan

N1 - Publisher Copyright: © 2026 American Chemical Society

PY - 2026/3/11

Y1 - 2026/3/11

N2 - Understanding the dynamic evolution of the aluminum anode interface in ionic liquid electrolytes is crucial for the large-scale application of rechargeable aluminum batteries (RABs). Herein, we use a series of advanced in situ characterizations to reveal a dendrite-to-corrosion transition, demonstrating that imidazolium cations (EMI+) fundamentally dominate anode degradation and instability. Therefore, based on a differential access mechanism, we engineer a metal–organic framework (MOF-C) layer with molecular-scale nanochannels that selectively block corrosive EMI + while accelerating AlCl4– diffusion. The modified Al/MOF-C anode achieves an unprecedented cycling stability of >11,000 h (at 1 mA cm–2 with minimal 20 mV overpotential) in symmetric cells, far exceeding all previous reports (typically <2000 h). Matched with natural graphite cathodes, full cells retain 95% capacity over 500 cycles. This work not only resolves the long-standing interfacial dispute in RABs but also establishes an ingenious solution aligned with interfacial evolution for next-generation stable metal anodes.

AB - Understanding the dynamic evolution of the aluminum anode interface in ionic liquid electrolytes is crucial for the large-scale application of rechargeable aluminum batteries (RABs). Herein, we use a series of advanced in situ characterizations to reveal a dendrite-to-corrosion transition, demonstrating that imidazolium cations (EMI+) fundamentally dominate anode degradation and instability. Therefore, based on a differential access mechanism, we engineer a metal–organic framework (MOF-C) layer with molecular-scale nanochannels that selectively block corrosive EMI + while accelerating AlCl4– diffusion. The modified Al/MOF-C anode achieves an unprecedented cycling stability of >11,000 h (at 1 mA cm–2 with minimal 20 mV overpotential) in symmetric cells, far exceeding all previous reports (typically <2000 h). Matched with natural graphite cathodes, full cells retain 95% capacity over 500 cycles. This work not only resolves the long-standing interfacial dispute in RABs but also establishes an ingenious solution aligned with interfacial evolution for next-generation stable metal anodes.

UR - https://www.scopus.com/pages/publications/105032349846

U2 - 10.1021/jacs.5c22732

DO - 10.1021/jacs.5c22732

M3 - Article

C2 - 41769918

AN - SCOPUS:105032349846

SN - 0002-7863

VL - 148

SP - 9990

EP - 10001

JO - Journal of the American Chemical Society

JF - Journal of the American Chemical Society

IS - 9

ER -