A Novel 4‐Fluorophenyl Isocyanate Additive Constructing Solid Cathodes‐Electrolyte Interface for High‐Performance Lithium‐Ion Batteries

Abstract Building a stable cathode‐electrolyte interface (CEI) is crucial for achieving high‐performance layered metal oxide cathode materials LiNi x Co y Mn 1‐x‐y O 2 (NCM). In this work, a novel 4‐fluorobenzene isocyanate (4‐FBC) electrolyte additive that contains isocyanate and benzene ring functional groups is proposed, which can form robust and homogeneous N‐rich and benzene ring skeleton CEI film on the cathode surface, leading to significant improvement in the electrochemical performance of lithium‐ion batteries. Taking LiNi 0.5 Co 0.2 Mn 0.3 O 2 (NCM523) as an example, the NCM523/SiO@Graphite pouch full cells with electrolytes containing a mass fraction of 1% 4‐FBC additives demonstrate improved capacity retention after 200 cycles, retaining capacity retention rates of 81.3%, which is much higher than that of 39.1% without additive. The improvement can be ascribed to the mitigation of electrolyte decomposition and inhibition of transition metal ions the dissolution from the cathode material due to the stable CEI film. Moreover, the electrochemical performance enhancement can also be achieved in high voltage and Ni‐rich cathode materials, indicating the universality and effectiveness of this strategy for the practical applications of high energy density lithium‐ion batteries.