Surface residual lithium compounds of Ni-rich cathodes are tremendous obstacles to electrochemical performance due to blocking ion/electron transfer and arousing surface instability. Herein, ultrathin and uniform Al2O3 coating via atomic layer deposition (ALD) coupled with the post-annealing process is reported to reduce residual lithium compounds on single-crystal LiNi0.6Mn0.2Co0.2O2 (NCM622). Surface composition characterizations indicate that LiOH is obviously reduced after Al2O3 growth on NCM622. Subsequent post-annealing treatment causes the consumption of Li2CO3 along with the diffusion of Al atoms into the surface layer of NCM622. The NCM622 modified by Al2O3 coating and post-annealing exhibits excellent cycling stability, the capacity retention of which reaches 92.2% after 300 cycles at 1 C, much higher than that of pristine NCM622 (34.8%). Reduced residual lithium compounds on NCM622 can greatly decrease the formation of LiF and the degree of Li+/Ni2+ cation mixing after discharge–charge cycling, which is the key to the improvement of cycling stability.

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