3D, Mutually Embedded MOF@Carbon Nanotube Hybrid Networks for High‐Performance Lithium‐Sulfur Batteries

Abstract Metal‐organic frameworks (MOFs) hybridized with a conductive matrix could potentially serve as a sulfur host for lithium‐sulfur (Li‐S) battery electrodes; so far most of the previously studied hybrid structures are in the powder form or thin compact films. This study reports 3D porous MOF@carbon nanotube (CNT) networks by grafting MOFs with tailored particle size uniformly throughout a CNT sponge skeleton. Growing larger‐size MOF particles to entrap the conductive CNT network yields a mutually embedded structure with high stability, and after sulfur encapsulation, it shows an initial discharge capacity of ≈1380 mA h g −1 (at 0.1 C) and excellent cycling stability with a very low fading rate. Furthermore, owing to the 3D porous network that is suitable for enhanced sulfur loading, a remarkable areal capacity of ≈11 mA h cm −2 (at 0.1 C) is obtained, which is much higher than other MOF‐based hybrid electrodes. The mutually embedded MOF@CNTs with simultaneously high specific capacity, areal capacity, and cycling stability represent an advanced candidate for developing high‐performance Li‐S batteries and other energy storage systems.