Abstract Metal–organic frameworks (MOFs) comprise coordination bonds and have attracted attention for electrochemical applications. However, MOFs are usually structurally weak in aqueous solutions, especially in acidic aqueous solutions, owing to their coordination bonds, making their application in charge-storage devices challenging. In the current work, we demonstrate a redox-active MOF (RAMOF) that is structurally stable and achieves reversible charge storage with almost the theoretical capacity even in acidic aqueous electrolytes owing to its strong Zr–O bonds and the large coordination number. In addition, the RAMOF exhibits high durability ( > 98% after 100 cycles) and high Coulombic efficiency (99.9%) owing to its high crystallinity and proton conductivity. An aqueous MOF–air rechargeable battery is fabricated and exhibits high durability and high Coulombic efficiency. Furthermore, the material recycling of the RAMOF based on its coordination bonds is demonstrated. Therefore, we conceptually prove the application and advantages of RAMOFs in aqueous environments.
Ryota Akai (2025) studied this question.