Tunable hierarchical porous carbon aerogel / graphene composites cathode matrix for Li-S batteries

It had been proven that carbon aerogel (CA) can effectively improve the conductivity of sulfur (S) and suppress the shuttle effect of polysulfides in Li-S batteries, due to its outstanding electrical conductivity and micropore-rich structure. However, the microstructure of CA was easy to collapse and shrink during carbonization, resulting in a dramatically drop in specific surface area and porosity. Herein, graphene nanosheets (GNs) were introduced in CA to reinforce the structural stability. As-prepared CA/GNs composites were fabricated from in-situ polymerization of resorcinol (R) and formaldehyde (F) in graphene oxide (GO) solution. It was found that the mass concentration of the GO solution had a significantly positive effect on hierarchical porous structure of the CA/GNs composites, which presented improve the electrochemical performances due to the combination of micro-, meso- and macro-pores. It is worth noting that the CA/GNs0.1 sample, obtained from 10 wt % GO solution, possessed the largest specific surface area of 665.477 m2 g−1 and the largest pore volume of 0.912 cm3 g−1. Especially, after incorporated with moderate amount of S (58.86 wt %), the CA/GNs0.1/S cathode exhibited the best electrochemical performances (initial discharging capacity of 1501 mAh g−1 at 0.1C and reversible capacities of 471 mAh g−1 after 100 cycles and 341 mAh g−1 after 500 cycles at 1C). This was attributed to the tunable hierarchical porous microstructure of the CA/GNs0.1 sample. Unfortunately, when increased the S content to 68.39 wt %, the electrochemical performance deteriorated in all aspects because of their sluggish reaction kinetics. These all results suggested that introducing GNs can feasibly enhance the performance of CA as matrix in Li-S batteries.