Large Organic Polar Molecules Tailored Electrode Interfaces for Stable Lithium Metal Battery

Abstract Lithium (Li) metal batteries (LMBs) are deemed as ones of the most promising energy storage devices for next electrification applications. However, the uneven Li electroplating process caused by the diffusion‐limited Li + transportation at the Li metal surface inherently promotes the formation of dendritic morphology and instable Li interphase, while the sluggish Li + transfer kinetic can also cause lithiation‐induced stress on the cathode materials suffering from serious structural stability. Herein, a novel electrolyte designing strategy is proposed to accelerate the Li + transfer by introducing a trace of large organic polar molecules of lithium phytate (LP) without significantly altering the electrolyte structure. The LP molecules can afford a competitive solvent attraction mechanism against the solvated Li + , enhancing both the bulk and interfacial Li + transfer kinetic, and creating better anode/cathode interfaces to suppress the side reactions, resulting in much improved cycling efficiency of LMBs. Using LP‐based electrolyte, the performance of LMB pouch cell with a practical capacity of ~1.5 Ah can be improved greatly. This strategy opens up a novel electrolyte designing route for reliable LMBs.