Stabilizing Nickel-Rich Cathodes in Aqueous Process via Nanochannel Water Confinement

Based on the two manuscripts provided, here is a possible abstract that summarizes the key findings:<br/><br/>Nickel-rich LiNi0.8Co0.1Mn0.1O2 (NMC 811) cathodes offer high voltage and capacity for high energy density lithium-ion batteries, but their manufacturing via aqueous electrode processing remains challenging due to material decomposition caused by the proton exchange reaction with water. This work addresses this issue by developing a protective nanocellulose coating on NMC 811 particles through electrostatic interactions. Wide-angle X-ray scattering measurements and atomistic simulations demonstrate that the nanochannels between nanocellulose chains can effectively confine interlayer water, preventing it from reaching the NMC surface. Density functional theory calculations predict that the functional groups of the nanocellulose exhibit stronger binding to the NMC surface than water molecules, suppressing Li+ surface segregation. As a result, nanocellulose-protected NMC electrodes prepared via aqueous processing exhibit higher capacity (133 vs. 59 mAh/g at 6C) and initial coulombic efficiency (83% vs. 62% at 0.1C) compared to unprotected electrodes. The optimized water-processed NMC electrodes also demonstrate superior rate capability and cycling stability compared to conventional NMP-based electrodes. This sustainable aqueous electrode manufacturing approach utilizing an in-situ formed nanocellulose barrier enables the realization of high-performance nickel-rich cathodes for next-generation lithium-ion batteries.