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migration of high-order LiPS toward Li (Supplementary Fig. 17) 42. The Li-S cell shows potential-vs.-capacity curves resembling those of the LiǀE_G2_0.5 M Li2S4ǀACFC_Li2S8 cell (Fig. 2). The presence of Li2S4 can be signified by the continuous potential dip at approximately 50 mAh gs_cathode−1 and by the high average CE of 99.0 % upon cycling. It is thus reasonable to postulate that the Li2S4-enabled solution pathway prevails in this Li-S cell. The initial discharge capacity is lower than that observed using ACFC, probably due to the capacity loss from uncontrollable diffusion of S62−. After 100 cycles, the cell can sustain the lower discharge plateau and deliver a specific capacity as high as 518 mAh g−1 based on Li2S8 preloaded in ECF cathode and 328 mAh g−1 based on the total sulfur from cathode and 0.5 M Li2S4 in electrolyte. Very few Li-S coin cells have been reported so far to survive for more than 40 cycles, with the continuous presence of the discharge plateau under similar conditions.43 The kinetics of the Li-S cell can be further improved by incorporation of a smart material (i.e., possessing high electronic conductivity and high Li+ transport) into the carbon matrix under lean electrolyte conditions.44 In summary, a solution-mediated pathway for sulfur reduction embracing synergetic chemical and electrochemical processes is described in Li-S cells with high sulfur loadings under lean electrolyte conditions. Excellent cycling performance of prototype Li-S cells validates the feasibility of developing practical Li-S cells using the Li2S4-retaining strategy. Data availability. Data supporting the finds of this study are available within the paper and its Supplementary Information file, and are available from the corresponding author upon reasonable request. Acknowledgements This work was supported as part of the Joint Center for Energy Storage Research, an Energy Innovation Hub funded by the U.S. Department of Energy (DOE), Office of Science, Basic Energy Sciences. Authors thank Dr. Nathan Canfield and Dr. Haiping Jia for SEM characterizations., Dr. Xiaolin Li for help on electrospinning setup, and Dr. Patrick Z El Khoury for help on Raman characterization. ACFC samples were kindly supplied by the Carbon Materials Division of Kuraray Co., Ltd, Japan. The depth-profile XPS measurements were performed at the Environmental Molecular Sciences Laboratory (EMSL), a national scientific user facility sponsored by the DOE Office of Biological and Environmental Research and located at Pacific Northwest National Laboratory. The operando XAS work at Advanced Light Source of Lawrence Berkeley National Laboratory was supported by the Director of the Office of Science, Office of Basic Energy Sciences, of DOE under contract no. DEAC02-05CH1123. We thank Dr. Sirine Fakra for her technical support at the beamline. Author contributions H.W. and J.-G.Z. conceived and designed the experiments. H.W. prepared electrolyte formulations, performed electrochemical measurements and fabricated cathode materials with Page 10 of 24PDF Image | A lithium-sulfur battery with a solution-mediated pathway
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