High Energy Density Lithium–Sulfur Batteries Based on Carbonaceous Two-Dimensional Additive Cathodes

[Image: see text] The increasing demand for electrical energy storage makes it essential to explore alternative battery chemistries that overcome the energy-density limitations of the current state-of-the-art lithium-ion batteries. In this scenario, lithium–sulfur batteries (LSBs) stand out due to the low cost, high theoretical capacity, and sustainability of sulfur. However, this battery technology presents several intrinsic limitations that need to be addressed in order to definitively achieve its commercialization. Herein, we report the fruitfulness of three different formulations using well-selected functional carbonaceous additives for sulfur cathode development, an in-house synthesized graphene-based porous carbon (ResFArGO), and a mixture of commercially available conductive carbons (CAs), as a facile and scalable strategy for the development of high-performing LSBs. The additives clearly improve the electrochemical properties of the sulfur electrodes due to an electronic conductivity enhancement, leading to an outstanding C-rate response with a remarkable capacity of 2 mA h cm(–2) at 1C and superb capacities of 4.3, 4.0, and 3.6 mA h cm(–2) at C/10 for ResFArGO(10), ResFArGO(5), and CAs, respectively. Moreover, in the case of ResFArGO, the presence of oxygen functional groups enables the development of compact high sulfur loading cathodes (>4 mg(S) cm(–2)) with a great ability to trap the soluble lithium polysulfides. Notably, the scalability of our system was further demonstrated by the assembly of prototype pouch cells delivering excellent capacities of 90 mA h (ResFArGO(10) cell) and 70 mA h (ResFArGO(5) and CAs cell) at C/10.