Metal–Organic-Framework-Derived 3D Hierarchical Matrixes for High-Performance Flexible Li–S Batteries

Lithium-sulfur (Li-S) batteries have shown exceptional theoretical energy densities, making them a promising candidate for next-generation energy storage systems. However, their practical application is limited by several challenging issues, such as uncontrollable Li dendrite growth, sluggish electrochemical kinetics, and the shuttling effect of lithium polysulfides (LiPSs). To overcome these issues, we designed and synthesized hierarchical matrixes on carbon cloth (CC) by using metal-organic frameworks (MOFs). ZnO nanosheet arrays were used as anode hosts (CC-ZnO) to enable stable Li plating and stripping. The symmetric cell with CC-ZnO@Li was demonstrated to have enhanced cycling stability, with a voltage hysteresis of ∼25 mV for over 800 h at 1 mA cm-2 and 1 mAh cm-2. To address the cathode challenges, we developed a multifunctional CC-NC-Co cathode host with physical confinement, chemical anchoring, and excellent electrocatalysis. The full cells with CC-ZnO@Li anodes and CC-NC-Co@S cathodes exhibited excellent electrochemical performance, with long cycling life (0.02% and 0.03% capacity decay per cycle when cycling 900 times at 0.5 C and 600 times at 1 C, respectively) and outstanding rate performance (793 mAh g-1 at 4 C). Additionally, the pouch cell based on the flexible CC-ZnO@Li anode and CC-NC-Co@S cathode showed good stability in different bending states. Overall, our study presents an effective strategy for preparing flexible Li and S hosts with hierarchical structures derived from MOF, which can pave the way for high-performance Li-S batteries.