Prompting structure stability of O3–NaNi0.5Mn0.5O2 via effective surface regulation based on atomic layer deposition

Abstract Layered O3 type oxides exhibit promising prospects as high-performance cathodes for sodium-ion batteries (SIBs) due to their low cost and high theoretical capacities. Nevertheless, the intrinsic surface composition and bulk structure degradation upon cycling presents a huge obstacle to stable sodium-ion storage/transportation. Besides, the effective surface decoration on layered O3 oxides is still challenging through conventional wet chemical route owing to their extraordinarily high surface sensitivities. Herein, a typical O3 type layered oxide of NaNi0.5Mn0.5O2 (NNMO) was selected and successfully encapsulated by precisely controlled Al2O3 layers via atomic layer deposition (ALD) technology. With the optimally controlled Al2O3 thickness of 3 nm, the surface regulated NNMO delivers a highly reversible capacity of 73.6 mA h g-1, with a significantly improved capacity retention of 68.0% after 300 cycles at 0.5 C, and a superior rate capability of 65.8 mA h g-1 at 10 C. Further air sensitivity tests demonstrate that the protective layer could effectively mitigate the generation of sodium-based impurities on NNMO, and reduce the surface sensitivities. Both chemical and electrochemical aging tests confirm the contribution of Al2O3 coating layer in alleviating ion dissolution as well as stabilizing the structure and morphology of NNMO. Based on regulating the surface of O3 type layered oxides utilizing ALD technique, this work supplies an effective and facile strategy to overcome the challenges from fast structure degradation and electrochemical property decay, which not only highlights the significance and effectiveness of surface engineering in secondary batteries, but also sheds light on accurate interface construction and regulation for active electrode materials, particularly for those sensitive to ambient atmosphere.