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 -