Chain-Transported Hypercoordinated Chloroaluminate Electrolyte for Solid-State Aluminum-Ion Batteries

作者：Ke Guo, Wei Wang, Handong Jiao, Wei‐Li Song, Shuqiang Jiao · 发表于：ACS Nano · 年份：2025 · DOI：10.1021/acsnano.5c09979 · 被引用次数：9 · 研究领域：Advanced Battery Materials and Technologies、Advancements in Battery Materials、Layered Double Hydroxides Synthesis and Applications

Aluminum-ion batteries (AIBs) have garnered significant attention due to their high safety and environmental compatibility. However, their practical development has been hindered by conventional liquid electrolytes, which suffer from a narrow electrochemical stability window and interfacial instability. Here, we develop a hypercoordinated chloroaluminate electrolyte (HCCAE) for low-cost and long-life solid-state AIBs, featuring a chain-assisted ion transport mechanism. Different from traditional ionic liquid electrolytes (ILs) that rely on AlCl 4 – and Al 2 Cl 7 – for ion conduction, the HCCAE forms a network where chloride ions from minimal 1-ethyl-3-methylimidazolium chloride (EMIC) migrate through a hypercoordinated AlCl 3 -rich framework, enabling a continuous, fast and stable solid-state conduction pathway [AlCl 3 –(AlCl 3 ) n –AlCl 3 –AlCl 4 – ]. The electrolyte exhibits ionic conductivity of 0.89 mS cm –1, an electrochemical window of >2.6 V, and electrolyte–electrode stability with Al plating/stripping over 900 h. The full battery demonstrates excellent cycling performance over 2000 cycles with high Coulombic efficiency. This work provides insights into ion transport mechanisms in aluminum-based solid electrolytes, which helps to achieve low-cost, high-safety, and long-life AIBs.