Engineering Configuration Compatibility and Electronic Structure in Axially Assembled Metal–Organic Framework Nanowires for High-Performance Lithium Sulfur Batteries

Both configuration match and electronic structure are vital for catalysts to efficiently promote the conversion of lithium polysulfides (LiPSs) in lithium–sulfur batteries (LSBs), which are however difficult to tailor in traditional catalysts that generally have a single active center. Herein, a series of dual-active-center MOFs (D-MOFs) were elaborated to manipulate the distance between different polar active sites and regulate the electronic structure of the metal center, which can match the configuration of long-chain LiPSs and optimize the metal–sulfur orbital hybridization. Moreover, in situ axial assembly of customized D-MOFs on carbon nanotubes delivers hierarchical sulfur hosts, which can remarkably improve the LSB performance, realizing high areal capacity (10.04 mAh cm–2) under high sulfur loading and lean electrolytes, and a pouch cell with high energy density (310.7 Wh kg–1). This work gives insight into the multiscale design of multifunctional catalytic MOFs, promising advancements in catalyst development for high-performance LSBs.