Having Your Cake and Eating It Too: Electrode Processing Approach Improves Safety and Electrochemical Performance of Lithium-Ion Batteries.

A layered Li[Ni x Co y Mn 1- x - y ]O 2 (NCM)-based cathode is preferred for its high theoretical specific capacity. However, the two main issues that limit its practical application are severe safety issues and excessive capacity decay. A new electrode processing approach is proposed to synergistically enhance the electrochemical and safety performance. The polyimide's (PI) precursor is spin-coated on the LiNi 0.5 Co 0.2 Mn 0.3 O 2 (NCM523) electrode sheet, and the homogeneous sulfonated PI layer is in situ produced by thermal imidization reaction. The PI-spin coated (PSC) layer provides improvements in capacity retention (86.47% vs 53.77% after 150 cycles at 1 C) and rate performance (99.21% enhancement at 5 C) as demonstrated by the NCM523-PSC||Li half-cell. The NCM523-PSC||graphite pouch full cell proves enhanced capacity retention (76.62% vs 58.58% after 500 cycles at 0.5 C) as well. The thermal safety of the NCM523-PSC cathode-based pouch cell is also significantly improved, with the critical temperature of thermal safety T 1 (the beginning temperature of obvious self-heating temperature) and thermal runaway temperature T 2 increased by 60.18 and 44.59 °C, respectively. Mechanistic studies show that the PSC layer has multiple effects as a passivation layer such as isolation of electrode-electrolyte contact, oxygen release suppression, solvation structure tuning, and the decomposition of carbonate solvents as well as LiPF 6 inhibition. This work provides a new path for a cost-effective and scalable design of electrode decoration with synergistic safety-electrochemical kinetics enhancement.