Model-Based Design of Graphite-Compatible Electrolytes in Potassium-Ion Batteries

Potassium-ion batteries (KIBs) are attractive alternatives to lithium-ion batteries (LIBs) because of their lower cost and global potassium sustainability. However, designing compatible electrolytes with graphite anode remains challenging. This is because the electrolyte decomposition and/or graphite exfoliation (due to K+–solvent co-insertion) always exist, which is much harder to overcome compared to the case of LIBs because of the higher activities of K+. Herein, we report a general principle to design compatible electrolytes with the graphite anode, where the K+ can be reversibly (de)intercalated. We find that the electrolyte composition is critical to determining the graphite performance, which can be tuned by the kind of solvent, anion, additives, and concentration. We present a new interfacial model to understand the variation in performance (i.e., K+ (de)intercalation or K+–solvent co-insertion or decomposition). Our model is distinctly different from the solid electrolyte interphase interpretation. This work offers new opportunities to design high-performance KIBs and potassium-ion sulfur batteries. Particularly, we present new guideline to design electrolytes for KIBs and other advanced mobile (ion) batteries.