Stabilizing the Li metal-electrolyte interface: Electrolyte design strategies and synergistic optimization

Abstract

Li metal batteries (LMBs), owing to their highest theoretical specific energy, are considered a crucial development direction for future high-energy-density battery systems. However, the high reactivity of the Li metal anode causes extreme electrochemical and chemical instability at its interface with the electrolyte. This instability triggers detrimental effects, including Li dendrite growth, repetitive cracking and reformation of the solid electrolyte interphase (SEI), and continuous irreversible consumption of both active Li and electrolyte. Therefore, designing high-performance electrolytes to precisely regulate interfacial chemistry has become one of the core strategies for advancing the practical application of LMBs. Significant progress has recently been made in stabilizing the Li metal-electrolyte interface (Li-electrolyte interface) through strategies including additives, weakly solvating electrolytes (WSE), high-concentration/localized high-concentration electrolytes (HCE/LHCE), and novel molecular design. Nevertheless, these advanced strategies and their corresponding stabilization mechanisms have not yet been systematically organized. To address this gap, this review focuses on four core electrolyte design strategies and systematically summarizes their mechanisms for stabilizing the Li-electrolyte interface. Building on this foundation, the inherent limitations of individual electrolyte design strategies are discussed. The analysis then focuses on the potential of synergistic electrolyte design to achieve a more electrochemically stable Li-electrolyte interface. Finally, future research directions requiring key focus are proposed for existing electrolyte design strategies.

Keywords

Li metal batteries / Solid electrolyte interphase / Li metal-electrolyte interface / Electrolyte design strategies / Synergistic optimization

RIGHTS & PERMISSIONS

Higher Education Press 2026

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