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

Abstract

Both configuration match and electronic structure are vital for catalyststo efficiently promotethe conversion of lithiumpolysulfides (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 (10.04mAhcm⁻²) under high sulfur loading and lean electrolytes, and a pouch cell with high energy density (310.7Wh kg⁻¹). This work gives insight into the multiscale design of multifunctional catalytic MOFs, promising advancements in catalyst development for high-performance LSBs.