Dimensionally Stable Polyimide Frameworks Enabling Long-Life Electrochemical Alkali-Ion Storage

Organic electrode materials hold unique advantages for electrochemical alkali-ion storage but cannot yet fulfill their potential. The key lies in the design of structurally stable candidates that have negligible solution solubility and can withstand thousands of cycles under operation. To this end, we demonstrate here the preparation of dimensionally stable polyimide frameworks from the two-dimensional cross-linking of tetraaminobenzene and dianhydride. The product consists of hierarchically assembled nanosheets with thin thickness and abundant porosity. Its robust molecular frameworks and advantageous nanoscale features render our polymeric material a promising cathode candidate for both sodium-ion and potassium-ion batteries. Most strikingly, an extraordinary cycle life of up to 6000 cycles at 2 A g–1 is demonstrated, outperforming most of its competitors. Theoretical simulations support the great activity of our polymeric product for the electrochemical alkali-ion storage.