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Prediction of battery aging with a detailed lithium plating model


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The efficient and fast charging of lithium-ion batteries remains one of the most delicate challenges for the automotive industry, being seriously affected by the formation of lithium metal on the surface of the negative electrode. At high states of charge, plating competes with and even replaces the intercalation reaction. Experimental evidences for plating include a voltage plateau due to lithium oxidation during discharge after plating, and a voltage drop due to re-intercalation of metallic lithium during heating of the cell.
In this presentation we will show that physicochemical models that explicitly include the plating reaction can predict these experimental observations, and can be used to predict plating limits as function of operating condition (temperature, charging current). To this goal, we include the plating reaction into a previously-developed [1] pseudo-3D model of a high-power lithium-ion pouch cell. An extensive literature research was carried out to identify accurate rate coefficients for the plating reaction, and validation was possible by comparison with experiments [2] in which the plating hints (voltage plateau and voltage drop) are present.
A relatively simple way to assess plating risk with physicochemical models is to compare the simulated local anode potential V_an with the thermodynamic plating condition of V_Li =0 V [3]. This approach has several pitfalls that have not been well discussed in literature. Firstly, the thermodynamics of the plating reaction depends on temperature and ion concentration. This means that V_Li is not constant equal to zero, as usually assumed, but depends on operating conditions. Secondly, we show that the kinetics of the plating reaction play a dominant role. Anode potentials V_an below V_Li do not necessarily induce plating if it is kinetically hindered. At low temperatures, which are usually seen to support plating, not only the main processes (intercalation and solid-state diffusion) become slow, but also the plating reaction itself becomes slow. Both effects are included in the present model.
As key output of parametric simulations, we present operation maps with quantitative plating amounts over a wide range of C-rates and temperatures (see Figure).

[1] S. Carelli, M. Quarti, M. C. Yagci, W. G. Bessler, „Modeling and Experimental Validation of a High-Power Lithium-Ion Pouch Cell with LCO/NCA Blend Cathode“ J. Electrochem. Soc. 166, A2990-A3003 (2019)
[2] M. Ecker, “Lithium Plating in Lithium-Ion batteries: An experimental and simulation approach”, PhD thesis, RWTH Aachen (2016).
[3] S. Carelli and W. G. Bessler, “Prediction of reversible lithium plating with a pseudo-3D lithium-ion battery model”, J. Electrochem. Soc. 167, 100515 (2020).

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