Abstract

Li-S chemistry is regarded as promising next-generation battery technology. However, its complex redox process and long-chain lithium polysulfides shuttling are hindering the development of practical Li-S battery technology. Various electrocatalysts are being investigated to address the problem by expediting reaction kinetics. Here we report Fe single metal atom catalyst (Fe-SAC) used in the sulfur cathode of Li-S batteries.Fe-SAC is synthesized using a modified metal-organic framework (MOF)-based approach, in which the low vapor pressure Fe element substitutes Zn during pyrolysis of ZIF-8 to attain Fe-N4 moieties by being coordinated with four substitutional nitrogen atoms in the graphene lattice. A freestanding 3D structure with Fe-SAC-functionalized carbon nanocages linked by a carbon nanofiber network is applied as the sulfur cathode scaffold. Here the nanocages are derived from Fe-doped ZIF with Fe-N4 SAC moieties embedded on the inside and outside surfaces. The carbon nanofiber network is derived from the carbonization of bacterial cellulose.We report several methods for assessing Fe-SAC catalytic function on sulfide redox reactions for the prepared electrode in cells with lithium polysulfides electrolytes. Electrochemical studies compare the performance of the nanostructured electrodes with or without Fe-SAC to confirm the catalytic effects in improving the Li-S battery performance. Accordingly, the prepared composite cathode delivers a high initial capacity of 1338 mAh/g at 0.1C and excellent rate capability at 2C with a reversible capacity of 840 mAh/g.

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