Enabling Aqueous Processing of Ni-Rich Layered Oxide Cathode Materials by Addition of Lithium Sulfate

Aqueous processing of Ni-rich layered oxide cathode materials is a promising approach to simultaneously decrease electrode manufacturing costs, while bringing environmental benefits by substituting the state-of-the-art (often toxic and costly) organic processing solvents. However, an aqueous environment remains challenging due to the high reactivity of Ni-rich layered oxides towards moisture, leading to lithium leaching and Al current collector corrosion because of the resulting high pH value of the aqueous electrode paste. Herein, a facile method was developed to enable aqueous processing of LiNi_0.8 Co_0.1 Mn_0.1 O₂ (NCM811) by the addition of lithium sulfate (Li₂ SO₄ ) during electrode paste dispersion. The aqueously processed electrodes retained 80 % of their initial capacity after 400 cycles in NCM811||graphite full cells, while electrodes processed without the addition of Li₂ SO₄ reached 80 % of their capacity after only 200 cycles. Furthermore, with regard to electrochemical performance, aqueously processed electrodes using carbon-coated Al current collector outperformed reference electrodes based on state-of-the-art production processes involving N-methyl-2-pyrrolidone as processing solvent and fluorinated binders. The positive impact on cycle life by the addition of Li₂ SO₄ stemmed from a formed sulfate coating as well as different surface species, protecting the NCM811 surface against degradation. Results reported herein open a new avenue for the processing of Ni-rich NCM electrodes using more sustainable aqueous routes.