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Predicting lithium-ion battery lifetime is one of the greatest unsolvedproblems in battery research right now. Recent years have witnessed a surge inlifetime prediction papers using physics-based, empirical, or data-drivenmodels, most of which have been validated against the remaining capacity(capacity fade) and sometimes resistance (power fade). However, there are manydifferent combinations of degradation mechanisms in lithium-ion batteries thatcan result in the same patterns of capacity and power fade, making itimpossible to find a unique validated solution. Experimentally, degradationmode analysis involving measuring the loss of lithium inventory, loss of activematerial at both electrodes, and electrode drift/slippage has emerged as astate-of-the-art requirement for cell degradation studies. In this paper wecoupled five degradation mechanisms together for the first time. We also showedhow three models with different levels of complexity can all fit the remainingcapacity and resistance well, but only the model with five coupled degradationmechanisms could also fit the degradation modes at all temperatures. This workproves that validating only against capacity and power fade is no longersufficient, and state-of-the-art experimental and modelling degradation studiesshould include degradation mode analysis for validation in the future.

Lithium-ion battery degradation: using degradation mode analysis to validate lifetime prediction modelling