Aluminum(Al)-organic batteries are considered as a great alternative option for next generation energy storage devices. The recent Al-organic batteries propose new storage mechanisms of cationic aluminum complex ([AlCl_x]^3−x, x ​= ​1 or 2) distinguished from traditional AlCl_4⁻, represent an important breakthrough for aluminum batteries. However, the electrochemical storage mechanisms (value of x in [AlCl_x]^3−x) are related to different types of organic materials, the poor cycling stability caused by inevitable dissolution of organic materials in electrolyte, and the complex synthetic process restrict the development of Al-organic batteries. Herein, polyimide (PI)/metal-organic frameworks (MOFs) hybrid material synthesizing from a facile one-pot strategy as cathode material in Al-organic battery is reported, providing with high specific capacity and excellent cycle stability. The PI/MOFs hybrid electrode achieves capacity of 83 ​mA ​h ​g⁻¹ ​at 1000 ​mA ​g⁻¹ with high coulombic efficiency (almost 100%). It also exhibits an excellent cycle performance of 1800 cycles with only a capacity decay of 0.0067% per cycle. Furthermore, the electrochemical storage mechanism of PI/MOFs is evaluated by ex-situ X-ray photoelectron spectroscopy and energy dispersive X-ray spectrum, which demonstrate that the cationic chloroaluminates interact with reduced carbonyl bonds in PI during discharge is AlCl₂⁺. These findings are of great significance for the basic understanding of the working mechanism of PI compound cathode in Al-organic batteries, which may serve as a solid foundation for further development of novel organic cathode materials and their composites for Al-organic batteries.

铝（Al）有机电池被认为是下一代储能设备的绝佳替代选择。最近的Al-有机电池提出阳离子铝络合物的新的存储机制（[的AlCl _X ] ^3-x，x = 1或2）由传统的AlCl区分_{4 ^-} ，代表铝的电池的一个重要突破。然而，电化学存储机制（[AlCl _x ] ^{3-x中x的值}）与不同类型的有机材料有关，由于有机材料不可避免地溶解在电解质中而导致循环稳定性差，并且复杂的合成过程限制了铝有机电池的发展。在此，报道了通过简单的一锅法作为铝有机电池的正极材料合成的聚酰亚胺（PI）/金属有机骨架（MOF）混合材料，具有高的比容量和优异的循环稳定性。PI / MOFs混合电极 在1000 mA g ^-1时达到83 mA h g ^-1的容量库仑效率高（几乎100％）。它还具有1800个循环的出色循环性能，每个循环的容量衰减仅为0.0067％。此外，通过异位X射线光电子能谱和能量色散X射线光谱对PI / MOFs的电化学存储机理进行了评估，结果表明，在放电过程中，阳离子氯铝酸盐与PI中还原的羰基键相互作用是AlCl ₂ ⁺。这些发现对于铝有机电池中PI复合阴极的工作机理的基本理解具有重要意义，为进一步开发新型有机铝材料及其有机阴极材料提供了坚实的基础。