CrP Nanocatalyst within Porous MOF Architecture to Accelerate Polysulfide Conversion in Lithium–Sulfur Batteries

Lithium-sulfur (Li-S) batteries demonstrate great potential for next-generation electrochemical energy storage systems because of their high specific energy and low-cost materials. However, the shuttling behavior and slow kinetics of intermediate polysulfide (PS) conversion pose a major obstacle to the practical application of Li-S batteries. Herein, CrP within a porous nanopolyhedron architecture derived from a metal-organic framework (CrP@MOF) is developed as a highly efficient nanocatalyst and S host to address these issues. Theoretical and experimental analyses demonstrate that CrP@MOF has a remarkable binding strength to trap soluble PS species. In addition, CrP@MOF shows abundant active sites to catalyze the PS conversion, accelerate Li-ion diffusion, and induce the precipitation/decomposition of Li₂S. As a result, the CrP@MOF-containing Li-S batteries demonstrate over 67% capacity retention over 1000 cycles at 1 C, ∼100% Coulombic efficiency, and high rate capability (674.6 mAh g^-1 at 4 C). In brief, CrP nanocatalysts accelerate the PS conversion and improve the overall performance of Li-S batteries.