An isothermal, multimodal, physics-based aging model for life prediction of Li-ion batteries is developed, for which a solvent-decomposition reaction leading to the growth of a solid electrolyte interphase (SEI) at the carbonaceous anode material is considered as the source of capacity fade. The rate of SEI film growth depends on both solvent diffusion through the SEI film and solvent-reduction kinetics at the carbon surface. The model is able to simulate a wide variety of battery aging profiles, e.g., open-circuit and constant-voltage storage, charge/discharge cycling, etc. An analysis of capacity-fade data from the literature reveals that the same set of aging parameters may be used for predicting cycling and constant-voltage storage. The use of this set of parameters for predicting storage under open-circuit voltage points out that part of the self-discharge is reversible.
The aging behavior of a commercial 2.3 Ah graphite/LFP cell during a year of cycling or storage at either 25 or 45 C is investigated. The performance decline of the cells during the aging period is monitored by non-destructive electrochemical techniques and is discussed in detail. An in-depth analysis of the aging results reveals that aging manifests itself more in terms of capacity loss rather than in terms of impedance increase, regardless of the cycling or storage conditions and of the temperature. The capacity fade is larger at 45 C than at 25 C, regardless of the cycling or storage conditions, and at a same temperature, cycling conditions are always more detrimental to capacity fade than storage conditions. The loss of cyclable lithium is identified as the main source of capacity fade in all cases, and for the cells aged at 45 C, a partial loss of graphite active material is suspected as well towards the end of the aging period.
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