Abstract

A high areal sulfur loading in a carbon-based cathode together with a high cell capacity is key to the design of lithium-sulfur batteries guaranteeing a superior energy density for use. However, a high sulfur loading produced using traditional blade coating techniques results in many technical issues such as sluggish electron/ion transport kinetics and cracking of the electrodes. Here a well designed two-step electrostatic spray deposition (ESD) technique is proposed to prepare a flexible, multilayer carbon electrode with a high sulfur areal loading, in which different carbon components by a careful selection are used for different functions in each layer. The unique "aerosol deposition" in the ESD creates buffer voids in the electrode, ensuring fast infiltration of the electrolyte and releasing the internal stress of the electrode thus avoiding the cracking of thick electrodes. With such an integrated design, the as-prepared cathode exhibits excellent flexibility, a long cyclic stability with a low capacity decay of 0.064% per cycle at 1 C for 500 cycles and a high rate capability of 736 mAh g−1 at 2 C. Moreover, a high areal sulfur loading of 9.4 mg cm−2 with an areal capacity of 6.2 mAh cm−2 at 0.1 C has been achieved.

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