Defect-Rich Amorphous Iron-Based Oxide/Graphene Hybrid-Modified Separator toward the Efficient Capture and Catalysis of Polysulfides

The sluggish sulfur reduction reaction, severe shuttle effect, and poor conductivity of sulfur species are three main problems in lithium-sulfur (Li-S) batteries. Functional materials with a strong affinity and catalytic effect toward polysulfides play a key role in addressing these issues. Herein, we report a defect-rich amorphous a-Fe₃O_4-x/GO material with a nanocube-interlocked structure as an adsorber as well as an electrocatalyst for the Li-S battery. The composition and defect structure of the material are determined by X-ray diffraction, high-resolution transmission electron microscopy, Raman spectroscopy, and X-ray photoelectron spectroscopy measurements. The distinctive open framework architecture of the as-engineered composite inherited from the metal-organic framework precursor ensures the stability and activity of the catalyst during extended cycles. The oxygen defects in the amorphous structure are capable of absorbing polysulfides and similarly work as catalytic centers to boost polysulfide conversion. Taking advantage of a-Fe₃O_4-x/GO on the separator surface, the Li-S battery shows a capacity over 610 mA h g^-1 at 1 C and a low decay rate of 0.12% per cycle over 500 cycles and superior rate capability. The functional material made via the low-cost synthesis process provides a potential solution for advanced Li-S batteries.