Covalent encapsulation of sulfur in a graphene/N-doped carbon host for enhanced sodium-sulfur batteries

Application of emerging room temperature sodium-sulfur (RT Na-S) battery is restrained by the poor conductivity, volume expansion of sulfur cathode and the shuttle effect of soluble polysulfides in electrolytes. Herein, an N-doped two-dimensional (2D) carbon host was derived from the polydopamine coated graphene for sulfur storage. Different from the conventional used melt-diffusion method to integrate sulfur on graphene layer physically, we employed a vapor-infiltration method to realize the homogenous incorporation of sulfur in the graphene-based host via C-S_x-C bond. A polydopamine-derived N-doped carbon layer was further coated on graphene to confine the high-temperature-induced gas-phase sulfur, which effectively increase the covalently bonded sulfur content in the host. Moreover, based on Time-of-Flight Secondary Ion Mass Spectrometry (TOF-SIMS) measurement, the C-S bonds are mainly formed beside N-doped carbon, being well explained by the stronger interaction between N-doped carbon and S₄ (sulfur vapor) than that of pure carbon from density functional theory (DFT) calculation results. When tested as a cathode for RT Na-S battery, the obtained N-doped graphene/sulfur cathode shows superior cycle stability.