Impact of Sulfur-Containing Additives on Lithium-Ion Battery Performance: From Computational Predictions to Full-Cell Assessments

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Electrolyte additives are pivotal for stabilization of lithium-ion batteries, by suppressing capacity loss through creation of an engineered solid-electrolyte-interphase-layer (SEI-layer) at the negative electrode and thereby increasing lifetime. Here, we compare four different sulfur-containing 5-membered-ring molecules as SEI-formers: 1,3,2-dioxathiolane-2,2-dioxide (DTD), propane-1,3-sultone (PS), sulfopropionic acid anhydride (SPA), and prop-1-ene-1,3-sultone (PES). Density functional theory calculations and electrochemical measurements both confirm appropriate reduction potentials. For a connection of the protective properties of the SEIs formed to the chemical structure of the additives, the decomposition paths are computed and compared with spectroscopic data for the negative electrode surface. The performance of full-cells cycled using a commercial electrolyte and the different additives reveals the formation of organic dianions to play a crucial beneficial role, more so for DTD and SPA than for P...