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In an ideal lithium-ion battery, apart from the intercalation and deintercalation of lithium ions between the positive and negative electrodes, no other side reactions occur, and there is no irreversible consumption of lithium ions. In an actual lithium-ion battery, side reactions exist all the time, and there is also irreversible consumption, such as electrolyte decomposition, dissolution of active materials, lithium metal deposition, etc., only to different extents. In an actual battery system, during each cycle, any side reaction that can generate or consume lithium ions or electrons may lead to a change in the capacity balance of the battery. Once the capacity balance of the battery changes, this change is irreversible and can accumulate through multiple cycles, having a serious impact on battery performance.

(1) Dissolution of Cathode Materials

The dissolution of Mn in spinel LiMn₂O₄ is the main reason for the reversible capacity attenuation of LiMn₂O₄. Regarding the dissolution mechanism of Mn, there are generally two explanations: the redox mechanism and the ion exchange mechanism. The redox mechanism means that at the end of the discharge, the concentration of Mn³⁺ is high, and the Mn⁴⁺ on the surface of LiMn₂O₄ will undergo a disproportionation reaction:

Mn⁴⁺ (solid) + Mn²⁺ (liquid) ⇌ 2Mn³⁺ (solid)

The divalent manganese ions generated by the disproportionation reaction dissolve in the electrolyte. The ion exchange mechanism means that Li⁺ and H⁺ exchange on the surface of the spinel, ultimately forming HMn₂O₄ which has no electrochemical activity.

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