Intrinsic Properties of Individual Inorganic Silicon-Electrolyte Interphase Constituents.

Because of the complexity, high reactivity, and continuous evolution of the silicon-electrolyte interphase (SiEI), "individual" constituents of the SiEI were investigated to understand their physical, electrochemical, and mechanical properties. For the analysis of these intrinsic properties, known SiEI components (i.e., SiO2, Li2Si2O5, Li2SiO3, Li3SiOx, Li2O, and LiF) were selected and prepared as amorphous thin films. The chemical composition, purity, morphology, roughness, and thickness of prepared samples were characterized using a variety of analytical techniques. On the basis of subsequent analysis, LiF shows the lowest ionic conductivity and relatively weak, brittle mechanical properties, while lithium silicates demonstrate higher ionic conductivities and greater mechanical hardness. This research establishes a framework for identifying components critical for stabilization of the SiEI, thus enabling rational design of new electrolyte additives and functional binders for the development of next-generation advanced Li-ion batteries utilizing Si anodes.