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2 Experimental work on lithium sulfide cathodes – materials and methods The experimental part of this work was carried out from 04/2012 to 05/2013 at Lawrence Berkeley National Laboratory1 under the supervision of Prof. Elton J. Cairns and in collaboration with his research group as well as the inorganic chemistry team at The Molecular Foundry2 and other members of the BATT program [60]. 2.1 The goal – coated lithium sulfide Lithium-sulfur cells have been studied for more than four decades. While the opti- mization of electrolytes, additives and counter-electrodes is critical for the long-term success of Li/S batteries, most research currently focuses on the design of the cath- ode’s microstructure. Many different approaches for optimizing it have been tried with some success, as discussed in several review articles [14, 30, 37, 61, 62]. Most conventional electrode designs suffer from poor cyclability, which has its ulti- mate cause in the mechanic stress induced by the swelling and shrinking of the active material during (de-)lithiation as well as side reactions of the dissolved polysulfides. Thus, a straightforward approach to mitigate degradation is to prevent polysulfide dissolution altogether. This can be achieved by a) choosing a gel or solid electrolyte with virtually no polysulfide solubility [63–66], or b) chemically modifying the elec- trode’s active surface so that sulfur is more strongly bound [67, 68], or c) introducing mechanical barriers on top of the electrode [69, 70] or inside the electrode [71, 72]. For the latter approach, carbon coatings have been suggested [71, 73], but conductive polymer coatings [72] have also been tried, as well as combinations thereof [74]. Of the above references, however, only [73] had been published at the time this work was started. The goal of this work is to prepare stable electrodes for Li/S cells synthesized from carbon-coated lithium sulfide. The coating around the active material, illustrated in Fig. 2.1, is intended to prevent direct contact between sulfur and the electrolyte, 1Environmental Energy Technologies Division, Lawrence Berkeley National Laboratory, 1 Cyclotron Road, Berkeley, CA 94720, USA 2The Molecular Foundry, Lawrence Berkeley National Laboratory, 1 Cyclotron Road, Berkeley, CA 94720, USA 17PDF Image | Lithium-Sulfur Battery: Design, Characterization, and Physically-based Modeling
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