Study of degradation mechanisms in aqueous-processed Ni-rich cathodes for enhanced sustainability of batteries

Traditionally, Ni-rich-layered oxide cathodes for lithium-ion batteries are produced utilizing N-methyl-2-pyrrolidone (NMP)-processed casting. However, to avoid using the reprotoxic solvent NMP, aqueous processing becomes one of the options. In this study, H₂O-processed LiNi_0.8Mn_0.1Co_0.1O₂ (NMC811) electrodes have been prepared to compare with the NMP-processed counterparts to investigate the degradation mechanism. The thick cathode-electrolyte interphase (CEI), NiO-like phase formation, and the growth of electrochemically inactive NMC particles after long-term cycling lead to capacity decay. In addition, phosphoric acid (H₃PO₄) was utilized to lower the pH value during the water-processed electrode preparation, to avoid corrosion of the aluminium current collector. The use of H₃PO₄ enhanced the capacity retention of NMC811 electrodes, likely owing to the formation of a LiF-rich CEI layer in the initial cycle(s) and the alleviated formation of electrochemically inactive NMC particles. Additionally, reaction inhomogeneity is present in H₃PO₄-modified electrodes, which is attributed to various Li-ion reinsertion resistances throughout the porous electrode during long-term cycling. Although the performance of the water-processed NMC811 electrode is not reaching the level of NMP-processed electrodes, this study provides key insights into the involved degradation mechanisms and demonstrates a viable pathway for the development of sustainable battery manufacturing processes.