Publication date: 10th April 2024
In the conventional view, electrode kinetic properties are obtained ex-situ near equilibrium, where the lithium concentration is only slightly perturbed. However, during high cycling rates, lithium transport within the electrode creates substantial lithium concentration differences, leading to dynamic phase separation. Therefore, we discovered that conventional kinetic properties fail to assess the effective rate capability at fast C-rates. Instead, kinetic phase heterogeneity, characterized by dynamic separation observed in-situ with X-ray diffraction (XRD) and deviations in lattice parameters, exclusively correlates with the capacity at high C-rate cycling.
To understand such phase evolution or separation, it is crucial to reveal the lithium transport pathway within the individual crystalline particles or grains. Using operando X-ray microscopy technology, our group has unveiled how lithium inserts and de-inserts within individual crystalline battery particles during cycling. We note that lithium transport and phase evolution behavior on the surface are critically different from those in the bulk and also play a crucial role in determining the rate capability.
By performing electrode-level operando XRD and single-particle-level operando X-ray microscopy, lithium insertion and de-insertion kinetics could be elucidated much further, aiding the understanding of fast battery cycling protocols.
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