Rapid synthesis of transition metal dichalcogenide-carbon aerogel composites for supercapacitor electrodes

Transition metal dichalcogenide (TMD) materials have recently demonstrated exceptional supercapacitor properties after conversion to a metallic phase, which increases the conductivity of the network. However, freestanding, exfoliated transition metal dichalcogenide films exhibit surface areas far below their theoretical maximum (1.2 %), can fail during electrochemical operation due to poor mechanical properties, and often require pyrophoric chemicals to process. On the other hand, pyrolyzed carbon aerogels exhibit extraordinary specific surface areas for double layer capacitance, high conductivity, and a strong mechanical network of covalent chemical bonds. In this paper, we demonstrate the scalable, rapid nanomanufacturing of TMD (MoS₂ and WS₂) and carbon aerogel composites, favoring liquid-phase exfoliation to avoid pyrophoric chemicals. The aerogel matrix support enhances conductivity of the composite and the synthesis can complete in 30 min. We find that the addition of transition metal dichalcogenides does not impact the structure of the aerogel, which maintains a high specific surface area up to 620 m² g^-1 with peak pore radii of 10 nm. While supercapacitor tests of the aerogels yield capacitances around 80 F g^-1 at the lowest applied currents, the aerogels loaded with TMD's exhibit volumetric capacitances up to 127% greater than the unloaded aerogels. In addition, the WS₂ aerogels show excellent cycling stability with no capacitance loss over 2000 cycles, as well as markedly better rate capability and lower charge transfer resistance compared to their MoS₂-loaded counterparts. We hypothesize that these differences in performance stem from differences in contact resistance and in the favorability of ion adsorption on the chalcogenides.