ScholarWorks@중앙대학교

초록

Electrolyte design dominated the safety and lifetime of lithium-ion batteries by determining both bulk ion transport and interfacial stability. This review organizes electrolyte development by the mechanistic classification including low-concentration electrolytes (LCEs), high- concentration electrolytes (HCEs), localized high-concentration electrolytes (LHCEs), weakly solvating electrolytes (WSEs), and high entropy electrolytes (HEEs). The electrolyte development had two central bottlenecks which were unstable interphases and sluggish bulk kinetics. Atomistic analysis using Density functional theory (DFT) and molecular dynamics (MD) simulations clarified solvation structures, nucleation pathways of interphases, and transport processes to solve the bottlenecks supported by experimental validation. HCEs approach developed from LCE enabled anion-derived inorganic interphases but increased viscosity. LHCEs restored conductivity while retaining HCEs-like interfacial chemistry, WSEs promoted anion-dominant solvation even at low salt concentration. Including the advantage of previous development, HEEs exploited configurational entropy to suppress clustering and extend operating conditions. The review also highlights machine learning potential (MLP) for interphase analysis as emerging methodologies that address the time and length scale limitations of conventional simulations while retaining quantum-level accuracy. Finally, the discussion outlines how atomic-scale simulations capture and interpret electrolyte mechanisms and emphasizes how simulation methodologies need to advance to provide deeper insight and reliable guidance for the discovery of next-generation electrolytes.

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