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Abstract The lithium-sulfur (Li/S) battery is a promising candidate for next-generation electro- chemical energy storage. Its unique combination of electrochemical performance, cost effectiveness, and environmental sustainability are unprecedented among battery ma- terials. As of today, however, Li/S batteries are only used for few niche applications; a broader adoption of this technology is impeded by the yet unsatisfactory energy effi- ciency, self discharge, and limited lifetime. This work contributes to the advancement of Li/S technology in two respects: First, a novel kind of positive electrode, based on coated lithium sulfide (Li2S), was prepared, tested and optimized. Second, the under- standing of the complex chemical and physical processes in the cell was improved by creating and utilizing a computational model of the Li/S battery. For the experimental part of this work, a chemical vapor deposition process was developed to apply a carbon coating to Li2S particles. The focus of this work was on the optimization of the process chain from commercially available chemicals to the final coin cell in general and on the characterization of the materials and electrodes during various processing steps in particular. For the modeling part, an existing multiscale electrochemical modeling framework was extended to enable full-cell simulations of Li/S batteries. The model includes a detailed description of electrochemistry, transport, and the evolution of solid phases in the cell, but also accounts for the electrical double layer and, in a generic fashion, the microstructure of the electrodes. Finally, a phenomenological description of the shuttle effect and associated cell degradation was implemented and analyzed. The parametrization and partial validation of the model makes use of original data col- lected for this purpose, but also data from literature. Simulation results comprise charge/discharge profiles, cyclic voltammetry, impe- dance spectra, and the evolution of the chemical composition of both the electrolyte and the electrodes over time. The analysis of these results reveals limiting factors and suggests improved operating conditions. The apt combination of theoretical and empirical methods enabled an improvement of the performance and cycle life of the novel cathode material, but also contributed to a more profound understanding of the Li/S battery. 9PDF Image | Lithium-Sulfur Battery: Design, Characterization, and Physically-based Modeling
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