ALD-Modified LiNi_0.33Mn_0.33Co_0.33O₂ Paired with Macroporous Silicon for Lithium-Ion Batteries: An Investigation on Lithium Trapping, Resistance Rise, and Cycle-Life Performance

Combining high energy density electrodes, such as silicon and NMC, has the potential to meet the growing demand of high energy electric vehicles. Herein, we report a full-cell design using a macroporous silicon anode and alumina-coated NMC cathode that provides stable cyclability by means of capacity-limited charging. The proposed Si-NMC full-cell design with alumina passivation on cathode has exhibited a stable capacity of 1000 mAh/g, with 1.2 times higher energy density than the Si-NMC full-cell without cathode passivation. The role of alumina coating on the altered half-cell electrode charging mechanisms and electrochemical full-cell reactions with Si anode was investigated systematically using various structural and chemical analyses. The alumina passivated Si-NMC full-cell designed in this study elucidated an interesting electrochemical behavior of Li trapping, which shed light on a significant pathway in the efficient utilization of Si-NMC battery for high energy applications.