Tunable Platform Capacity of Metal–Organic Frameworks via High-Entropy Strategy for Ultra-Fast Sodium Storage

Abstract Precise regulation of the platform capacity/voltage of electrode materials contributes to the efficient operation of sodium-ion fast-charging devices. However, the design of such electrode materials is still in a blank stage. Herein, based on tunable metal–organic frameworks, we have designed a novel material system—two-dimensional high-entropy metal–organic frameworks (HE-MOFs), which exhibits unique properties in sodium storage and is of vital importance for realizing fast-charging batteries. Furthermore, we have found that the high-entropy effect can regulate the electronic structure, the sodium-ion migration environment, and the sodium-ion storage active sites, thereby meeting the requirements of electrode materials for sodium-ion fast-charging devices. Impressively, the HE-MOFs material still maintains a reversible specific capacity of 89 mAh g −1 at a current density of 20 A g −1 . It presents an ideal sodium storage voltage plateau of approximately 0.5 V, and its platform capacity is increased to 122.7 mAh g −1 , far superior to that of Mn-MOFs (with no platform capacity). This helps to reduce safety hazards during the fast-charging process and demonstrates its great application value in the fields of fast-charging sodium-ion batteries and capacitors. Our research findings have broken the barriers to the application of non-conductive MOFs as energy storage materials, enhanced the understanding of the regulation of platform capacity and voltage, and paved the way for the realization of high-security sodium-ion fast-charging devices.