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In order to develop long-lifespan batteries, it is of utmost importance to identify the relevant aging mechanisms and their relation to operating conditions. The capacity loss in a lithium-ion battery originates from (i) a loss of active electrode material and (ii) a loss of active lithium. The focus of this work is the capacity loss caused by lithium loss, which is irreversibly bound to the solid electrolyte interface (SEI) on the graphite surface. During operation, the particle surface suffers from dilation, which causes the SEI to break and then be rebuilt, continuously. The surface dilation is expected to correspond with the well-known graphite staging mechanism. Therefore, a high-power 2.6 Ah graphite/LiNiCoAlO2 cell (Sony US18650VTC5) is cycled at different, well-defined state-of-charge (SOC) ranges, covering the different graphite stages. An open circuit voltage model is applied to quantify the loss mechanisms (i) and (ii). The results show that the lithium loss is the dominant cause of capacity fade under the applied conditions. They experimentally prove the important influence of the graphite stages on the lifetime of a battery. Cycling the cell at SOCs slightly above graphite Stage II results in a high active lithium loss and hence in a high capacity fade.

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