Enhancing the High-Voltage Cycling Performance of LiNi_0.5Mn_0.3Co_0.2O₂ by Retarding Its Interfacial Reaction with an Electrolyte by Atomic-Layer-Deposited Al₂O₃

Abstract

High-voltage (>4.3 V) operation of LiNi(x)Mn(y)Co(z)O2 (NMC; 0 ≤ x, y, z < 1) for high capacity has become a new challenge for next-generation lithium-ion batteries because of the rapid capacity degradation over cycling. In this work, we investigate the performance of LiNi(0.5)Mn(0.3)Co(0.2)O2 (NMC532) electrodes with and without an atomic-layer-deposited (ALD) Al2O3 layer for charging/discharging in the range from 3.0 to 4.5 V (high voltage). The results of the electrochemical measurements show that the cells with ALD Al2O3-coated NMC532 electrodes have much enhanced cycling stability. The mechanism was investigated by using X-ray photoelectron spectroscopy, X-ray absorption spectroscopy, and electrochemical methods. We find that the ultrathin ALD Al2O3 film can reduce the interface resistance of lithium-ion diffusion and enhance the surface stability of NMC532 by retarding the reactions at NMC532/electrolyte interfaces for preventing the formation of a new microstructure rock-salt phase NiO around the NMC532 surfaces.