The electrochemical performance deterioration mechanism of LiNi0.83Mn0.05Co0.12O2 in aqueous slurry and a mitigation strategy

Integrating high-nickel layered oxide cathodes with aqueous slurry electrode preparation routes holds the potential to simultaneously meet the demands for high energy density and low-cost production of lithium-ion batteries. However, the influence of dual exposure to air and liquid water as well as the heating treatment during aqueous slurry electrode processing on the high-nickel layered oxide electrode is yet to be understood. In this study, we systematically investigate the structural evolution and electrochemical behaviors when LiNi_0.83Mn_0.05Co_0.12O₂ (NMC83) is subjected to aqueous slurry processing. It was observed that the crystal structure near the surface of NMC83 is partially reconstructed to contain a mixture of rock-salt and layered phases when exposed to water, leading to the deteriorated rate capability of the NMC83 electrodes. This partial surface reconstruction layer completely converts into a pure rock-salt phase upon cycling, accompanied by the release of O₂, Ni leaching, catalyzed decomposition of the electrolyte, and the formation of a thick cathode electrolyte interphase layer. The byproducts of the electrolyte and dissolved Ni could shuttle to the Li metal side, causing a crosstalk effect that results in a thick and unstable solid electrolyte interphase layer on the Li surface. These in combination severely undermined the cycling stability of the NMC83 electrodes obtained from the aqueous slurry. A mitigation strategy using molecular self-assembly technique was demonstrated to enhance the surface stability of water-treated NMC83. Our findings offer new insights for tailoring ambient environment stability and aqueous slurry processability for ultra-high nickel layered oxide and other water-sensitive cathode materials.