Ordered Mesoporous Graphitic Carbon/Iron Carbide Composites with High Porosity as a Sulfur Host for Li–S Batteries

The lithium–sulfur battery (LSB) is a promising candidate for future energy storage but faces technological challenges including the low electronic conductivity of sulfur and the solubility of intermediates during cycling. Additionally, current host materials often lack sufficient conductivity and porosity to raise the sulfur loading to over 80 wt %. Here, ordered mesoporous graphitic carbon/iron carbide nanocomposites were prepared via an evaporation-induced self-assembly process using soluble resol, prehydrolyzed tetraethyl orthosilicate (TEOS), and iron(III) chloride as the carbon, silica (SiO2), and iron precursors, respectively. Graphitization and SiO2 etching were conducted simultaneously via Teflon-assisted, solid-state decomposition at high temperature. A high surface area (∼3100 m2 g–1), large pore volume (∼3.3 cm3 g–1), and graphitized carbon frame were achieved, giving a high sulfur loading (85 wt %) while tolerating volumetric expansion during discharge. Electrochemical testing of a LSB containing the composite/sulfur cathode exhibited a superior reversible capacity exceeding 1300 mAh g–1 at a moderate current (C/10) and a low decay in capacity of 9% after 500 cycles at C/5. The interaction between mesoporous graphitic carbon and sulfur is proposed.