Tailoring iron hexadecafluorophthalocyanine/GO nanocomposite separators for polysulfide adsorption and enabling fast electrochemical kinetics of Li-S batteries

The cycling stability of lithium-sulfur batteries is significantly compromised by the shuttle effect. Herein, we employed a preformed process to successfully load spherical nanoparticles of Iron hexadecafluorophthalocyanine (FePcF16) with sizes between 10 and 20 nm onto oxidized graphene sheets. The FePcF16 spherical particles with lithium and sulfur-affinitive sites maximally expose catalytically active sites, facilitating effective adsorption and catalysis of polysulfides (LiPSs). Density-functional theory (DFT) calculations suggest that the electron-rich fluorine substituents enhance the conjugation effect of FePcF16, facilitating electronic communication between the catalyst and graphene oxide (GO), achieving precise modulation of the electronic structure of Fe-N-4 active centers. The electrochemical analysis demonstrates that the nanostructured and Fe-N-4 site-containing FePcF16 integrated with the robust two-dimensional graphene structure synergistically facilitates both redox reactions and lithium affinity effects. Consequently, in extended cycling tests at 2 C, the initial discharge-specific capacity reached 857.7 mAh g(-1). After 500 cycles, the capacity remained at 737.7 mAh g(-1), with a minimal capacity decay rate of only 0.028 % per cycle.