Chemical Roadmap toward Stable Electrolyte–Electrode Interfaces in All-Solid-State Batteries

All-solid-state batteries (ASSBs) hold significant promise for enhanced safety, energy density, and power density compared to conventional lithium-ion batteries. However, their development is impeded by the growth of resistance and diminished cell performance due to the interfacial reactivity between the electrodes and solid-state electrolytes. Comprehensive knowledge of interface reactions and effective mitigation strategies are essential to unlock the potential of ASSBs. Herein, we introduce the concept of a stability network to encode chemical and electrochemical reactions among lithium and non-lithium compounds within a comprehensive and complex network structure. Through analyzing the topological structure of the stability network, we reveal an organized and chemically instructive pattern of two-phase reactions and equilibria under different electrochemical conditions. This understanding of intrinsic patterns in relation to compositional, chemical, and electrochemical variables offers a set of principles for the experimental design and engineering of interfaces, serving as a chemical roadmap for achieving stable electrolyte–electrode interfaces in ASSBs.