Atomic Insights into the Fundamental Interactions in Lithium Battery Electrolytes

作者：Xiang Chen, Qiang Zhang · 发表于：Accounts of Chemical Research · 年份：2020 · DOI：10.1021/acs.accounts.0c00412 · 被引用次数：365 · 研究领域：Advanced Battery Materials and Technologies、Advancements in Battery Materials、Advanced Battery Technologies Research

Conspectus Building high-energy-density batteries is urgently demanded in contemporary society because of the continuous increase in global energy consumption and the quick upgrade of electronic devices, which promotes the use of high-capacity lithium metal anodes and high-voltage cathodes. Achieving a stable interface between electrolytes and highly reactive electrodes is a prerequisite to constructing a safe and powerful battery, in which electrolyte regulation plays a decisive role and largely determines the long-term and rate performances. The bulk and interfacial properties of electrolytes are directly determined by the fundamental interactions and the as-derived microstructures in electrolytes. Different from experimental trial-and-error approaches, the rational bottom-up design of electrolytes based on a comprehensive and deep understanding of the fundamental interactions between electrolyte compositions and the structure–function relationship is highly expected to accelerate breaking through the bottleneck in current technology and realizing next-generation Li batteries. In this Account, we afford an overview of our recent attempts toward rational electrolyte design for safe Li batteries based on a comprehensive understanding of the cation–solvent, cation–anion, and anion–solvent interactions in electrolytes. The formation of cation–solvent complexes decreases the reductive stability but increases the oxidative stability of solvent molecules according to frontier mole...