3-D vertically aligned few layer graphene - partially reduced graphene oxide/sulfur electrodes for high performance lithium-sulfur batteries

3-D vertically aligned few-layered graphene (FLGs) nanoflakes synthesised using microwave plasma enhanced chemical vapour deposition are melt-impregnated with partially reduced graphene oxidesulfur (PrGO-S) nanocomposites for use in lithium-sulfur batteries. The aligned structure and the presence of interconnected micro voids/channels in the 3-D FLG/PrGO-S electrodes serves as template not only for the high sulfur loading (up to 80 wt%, areal loading of 1.2mg cm(-2)) but also compensates for the volume changes occurring during charge-discharge cycles. The inter-connectivity of the electrode system further facilitates fast electronic and ionic transport pathways. Consequently, the binder-free 3-D FLG/PrGO-S electrodes display a high first-cycle capacity (1320 mA h g(-1) at C/20), along with excellent rate capability of similar to 830mA h g(-1) and 700 mA h g(-1) at 2C and 5C rates, respectively. The residual functional groups of PrGO (-OH, -C-O-C-and -COOH) facilitate fast and reversible capture of Li+ ions while confining the polysulfide shuttles, thus, contributing to excellent cycling capability and retention capacity. The 3D electrodes demonstrate excellent capacity retention of similar to 80% (1040 mA h g(-1) at C/10) over 350 charge-discharge cycles. Comparatively, the 2-D planar PrGO-S electrodes displayed poor electronic conductivity and can only provide 560 mA h g(-1) after 150 cycles, thereby further highlighting the vital role of the electrode morphology in improving the electrochemical performance of Li-S batteries.