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A lithium-sulfur battery with a solution-mediated pathway

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A lithium-sulfur battery with a solution-mediated pathway ( a-lithium-sulfur-battery-with-solution-mediated-pathway )

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A lithium-sulfur battery with a solution-mediated pathway operating under lean electrolyte conditions Hui Wang1,2, Yuyan Shao1,2, Huilin Pan1,2, Xuefei Feng3, Ying Chen1,4, Yi-Sheng Liu3, Eric D Walter4, Mark H. Engelhard5, Kee Sung Han1,4, Tao Deng2, Guoxi Ren3, Dongping Lu2, Xiaochuan Lu2, Wu Xu2, Chunsheng Wang6, Jun Feng3, Karl T. Mueller1,4, Jinghua Guo3, Kevin R. Zavadil6, and Ji-Guang Zhang1,2* 1. Joint Center for Energy Storage Research (JCESR), Pacific Northwest National Laboratory, Richland, WA 99354, USA 2. Energy & Environment Directorate, Pacific Northwest National Laboratory, Richland, Washington 99354, USA 3. Advanced Light Source, Lawrence Berkeley National Laboratory, Berkeley, CA 94720, USA. 4. Physical and Computational Sciences Directorate, Pacific Northwest National Laboratory, Richland, Washington 99354, USA 5. Environmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory, Richland, Washington 99354, USA 6. Joint Center for Energy Storage Research (JCESR), Sandia National Laboratories, PO BOX 5800, Albuquerque, New Mexico 87185, USA. Corresponding author: J.-G. Zhang, jiguang.zhang@pnnl.gov Abstract Lithium-sulfur (Li-S) battery is one of the most promising candidates for the next generation energy storage systems. However, several barriers, including polysulfide shuttle effect, the slow solid-solid surface reaction pathway in the lower discharge plateau, and corrosion of Li anode still limit its practical applications, especially under the lean electrolyte condition required for high energy density. Here, we propose a solution-mediated sulfur reduction pathway to improve the capacity and reversibility of the sulfur cathode and suppress dendrite growth on the Li metal anode simultaneously. With this method, a high coulombic efficiency (99%) and stable cycle life over 100 cycles were achieved under application-relevant conditions (S loading: 6.2 mg cm-2; electrolyte to sulfur ratio: 3 mLE gs-1; sulfur weight ratio: 72 wt%). This result is enabled by a specially designed Li2S4-rich electrolyte, in which Li2S is formed through a chemical disproportionation reaction instead of electrochemical routes. A diglyme solvent was used to obtain electrolytes with the optimum range of Li2S4 concentration. Operando X-ray absorption spectroscopy confirms the solution pathway in a practical Li-S cell. This solution pathway not only introduces a new electrolyte regime for practical Li-S batteries, but also provides a new perspective for bypassing the inefficient surface pathway for other electrochemical processes. Page 1 of 24

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