In Situ Characterizations of the Dynamics of Cathode Electrolyte Interfaces at Different Current Densities

Abstract LiNi_0.8Mn_0.1Co_0.1O₂ with high nickel content plays a critical role in enabling lithium metal batteries (LMBs) to achieve high specific energy density, making them a prominent choice for electric vehicles (EVs). However, ensuring the long‐term cycling stability of the cathode electrolyte interfaces (CEIs), particularly at fast‐charge conditions, remains an unsolved challenge. The decay mechanism associated with CEIs and electrolytes in LMB at high current densities is still not fully understood. To address this issue, in situ Fourier transform infrared (FTIR) is employed to observe the dynamic process of formation/disappearance/regeneration of CEIs during charge and discharge cycles. These dynamic processes further exacerbate the instability of CEIs as current density increases, leading to rupture and dissolution of CEIs and subsequent deterioration in battery performance because of continuous electrolyte reactions. Additionally, the dynamic changes occurring within individual components of CEIs at different cycling stages and various current densities are also discussed. The results demonstrate that excellent capacity retention at small current density is attributed to enrichment of inorganic compounds (Li₂CO₃, LiF, etc.) and rendering better stability and smaller expansion of CEIs. The key to achieving excellent electrochemical performance at high current densities lies on protecting CEIs, mainly inorganic components.