Although lithium-sulfur (Li-S) batteries have long been touted as next-generation energy storage devices, the rampant dendrite growth at the anode side and sluggish redox kinetics at the cathode side drastically impede their practical application. Herein, a dual-functional fibrous skeleton implanted with single-atom Co-Nx dispersion is devised as an advanced modificator to realize concurrent regulation of both electrodes. The rational integration of single-atomic Co-Nx sites could convert the fibrous carbon skeleton from lithiophobic to lithiophilic, helping assuage the dendritic formation for the Li anode. Meanwhile, the favorable electrocatalytic activity from the Co-Nx species affording a lightweight feature effectively enables expedited bidirectional conversion kinetics of sulfur electrochemistry, thereby inhibiting the polysulfide shuttle. Moreover, the interconnected porous framework endows the entire skeleton with good mechanical robustness and fast electron/ion transportation. Benefiting from the synergistic effects between atomically dispersed Co-Nx sites and three-dimensional conductive networks, the integrated Li-S full batteries can achieve a reversible areal capacity (>7.0 mAh cm-2) at a sulfur loading of 6.9 mg cm-2. This work might be beneficial to the development of practically viable Li-S batteries harnessing single-atom mediators.
Keywords: Li−S batteries; dendrite inhibition; dual-functional; polysulfide conversion; single-atomic Co−Nx.