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

D. P. Singh, N. Soin, S. Sharma, S. Basak, S. Sachdeva, S. S. Roy, H. W. Zanderbergen, J. A. McLaughlin, M. Huijben, M. Wagemaker

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    3-D vertically aligned few-layered graphene (FLGs) nanoflakes synthesised using microwave plasma enhanced chemical vapour deposition are melt-impregnated with partially reduced graphene oxide-sulfur (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 1.2 mg 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 ∼830 mA 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 ∼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.

    Original languageEnglish
    Pages (from-to)1516-1523
    Number of pages8
    JournalSustainable Energy and Fuels
    Issue number7
    Publication statusPublished - 13 Jul 2017


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