Cycling capacity recovery effect: A coulombic efficiency and post-mortem study

Abstract The analysis of lithium-ion battery aging relies on correct differentiation between irreversible and reversible capacity changes. Anode overhang regions have been observed to influence Coulombic Efficiency (CE) measurements through lithium diffusion into and out of these areas, complicating precise capacity determination. This work presents an analysis of the extent of graphite anode overhang lithiation after calendar storage by means of local X-ray diffraction (XRD), CE measurements, and color change analysis. We found LiC 12 lithiation of the anode overhang area after 20 month storage at 40 °C at high state of charge (SoC) and partial lithiation (LiC 18 ) at medium SoC storage at 40 °C and 25 °C. Graphite color changes in the overhang areas are observed and consistent with the state of lithiation measured by XRD. Coulombic efficiencies greater than unity and increasing capacity during 1200 h of cycling are detected for high SoC storage cells. The capacity difference between high and low storage SoC batteries decreases by up to 40 mAh (3.6% of nominal capacity) after cycling compared to tests directly after storage. Consequently, the size of the anode overhang areas as well as the battery storage temperature and duration need to be considered in CE analysis and state of health assessment.

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