Further enhancement in the energy densities of rechargeable lithium batteries calls for novel cell chemistry with advanced electrode materials that are compatible with suitable electrolytes without compromising the overall performance and safety, especially when considering high‐voltage applications. Significant advancements in cell chemistry based on traditional organic carbonate‐based electrolytes may be successfully achieved by introducing fluorine into the salt, solvent/cosolvent, or functional additive structure. The combination of the benefits from different constituents enables optimization of the electrolyte and battery chemistry toward specific, targeted applications. This Review aims to highlight key research activities and technical developments of fluorine‐based materials for aprotic non‐aqueous solvent‐based electrolytes and their components along with the related ongoing scientific challenges and limitations. Ionic liquid‐based electrolytes containing fluorine will not be considered in this Review.

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Perspective on recent improvements in experiment and theory towards realizing lithium metal electrodes with liquid electrolytes.

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The tris(trimethylsilyl) phosphite (TMSPi) is considered as an ideal electrolyte additive for lithium ion batteries. In this work, its positive effect as well as its failure mechanism in a LiPF 6 containing electrolyte was studied by means of selected electrochemical, structural and analytical techniques. The LiNi 0.5 Co 0.2 Mn 0.3 O 2 /graphite cells with TMSPi as electrolyte additive were cycled between 2.8 and 4.6 V.Thanks to the compact cathode electrolyte interphase formed by the oxidative decomposition of TMSPi in a freshly prepared TMSPi containing electrolyte, both the discharge capacity and the cycling stability of cells were enhanced. However, our results also show that TMSPi actually reacts with LiPF 6 at room temperature. TMSPi is consumed by this spontaneous reaction after aging for certain time. In addition, a part of the fluorophosphates, generated from the hydrolysis of LiPF 6 , is bonded to one or two TMS groups, causing a decrease in the fluorophosphate content in the CEI film. Consequently, the cycling stability of the lithium ion cells with aged TMSPi containing electrolyte deteriorates. The obtained results offer important insights into the practical application of TMSPi, which means that TMSPi can only be used as an effective additive in a freshly prepared LiPF 6 containing electrolyte.

Application of different electrolyte components as blends in nonaqueous electrolyte formulations represents a viable approach towards improving the overall performance and reliability of a lithium ion battery cell. By combining the advantages of different electrolyte constituents, cell chemistry can be optimized and tailored for a specific purpose. In this paper, the current progress on possibilities, advantages, as well as limitations of blended nonaqueous electrolyte formulations, including solvent, salt and additive blends is reviewed and discussed. Emphasis is set on the physicochemical, electrochemical, and safety aspects. In addition, the aim of this review is to provide perspective and possible strategy for further and future development of blended nonaqueous electrolytes with long life, high energy density, high power, and adequate safety at competitive manufacturing costs. The provided overview and perspective on blended nonaqueous electrolyte formulations should encourage researchers to proceed with further and deeper investigations in this promising field of advanced batteries.