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.