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The study focuses on NMC811, a promising material for high-capacitybatteries, and investigates the challenges associated with its use,specifically the formation of the Cathode Electrolyte Interphase (CEI) layerdue to chemical reactions. This layer is a consequence of the position of theLUMO energy level of NMC811 that is close to the HOMO level of liquidelectrolyte, resulting in electrolyte oxidation and cathode surface alterationsduring charging. A stable CEI layer can mitigate further degradation byreducing the interaction between the reactive cathode material and theelectrolyte. Our research analyzed the CEI layer on NMC811 using advancedtechniques such as 4D-STEM ACOM and STEM- EDX, focusing on the effects ofdifferent charging voltages (4.3 V and 4.5 V). The findings revealed varyingdegrees of degradation and the formation of a fluorine-rich layer on thesecondary particles. Detailed analysis showed the composition of this layerdiffered based on the voltage: only LiF at 4.5 V and a combination of LiF andLiOH at 4.3 V. Despite LiF's known stability as a CEI protective layer, ourobservations indicate it does not effectively prevent degradation in NMC811.The study concludes that impurities and unwanted chemical reactions leading tosuboptimal CEI formation are inevitable. Therefore, future efforts should focuson developing protective strategies for NMC811, such as the use of specificadditives or coatings.

Investigating Cathode Electrolyte Interphase Formation in NMC 811 Primary Particles Through Advanced 4D-STEM ACOM Analysis