Reversible Self-discharge of LFP/Graphite and NMC811/Graphite Cells Originating from Redox Shuttle Generation

Unwanted parasitic reactions in lithium-ion cells lead to self-discharge and inefficiency, especially at high temperatures. To understand the nature of those reactions this study investigates the open circuit storage losses of LFP/graphite and NMC811/graphite pouch cells with common alkyl carbonate electrolytes. The cells perform a storage test at 40 °C with a 500 h open circuit period after formation at temperatures between 40 °C and 70 °C. Cells formed at elevated temperature showed a high reversible storage loss that could be assigned to a redox shuttle generated in the electrolyte during formation. A voltage hold after formation can reduce the shuttle-induced self-discharge as indicated by significantly lower reversible storage losses, the absence of shuttling currents in cyclic voltammetry and improved metrics in ultra-high precision cycling. The addition of two weight percent vinylene carbonate can prevent redox shuttle generation and leads to almost zero reversible self-discharge.