Interfacial
reaction mechanisms at the anode/separator interface
play a central role in the performance and safety of lithium-ion batteries
during fast charging. We report a mechanistic study on the evolution
and interactions of the aging mechanisms at the anode/separator interface
in lithium cobalt oxide/graphite pouch cells charged with variable
charging rates (1–6C) over 10 cycles. In situ electrochemical measurements, including voltage relaxation, Coulombic
efficiency, and direct current internal resistance, indicated an incremental
lithium loss until the C rates were ≤5C. A substantial capacity
fade is observed in the first few cycles of fast charging, but the
magnitude of capacity fade progressively diminishes with the number
of cycles, indicating a suppression in the lithium deposition mechanism.
Post-mortem film thickness, X-ray photoelectron spectroscopy (XPS),
and scanning electron microscopy (SEM) analyses were performed to
elucidate the evolution of electrolyte decomposition, the solid–electrolyte
interface (SEI), lithium plating, and film fracture mechanisms with
C rate. XPS measurements confirmed an increasing lithium concentration
in an SEI film with an increase in the C rate. SEM images showed a
growth of dendritic lithium on the anode surface from 1C to 3C. Precrack
formation leading to an interfacial film fracture was observed at
higher C rates. A differential analysis of the discharge capacity
indicated a possible two-phase delithiation from the anode and reduced
cathodic lithiation due to lithium loss at high C rates.