O3-type layered oxides hold significant promise as the material for cathodes in sodium-ion batteries for their favorable electrochemical properties, while irreversible structural degradation and harmful phase transitions during cyclic operation limit the practical application of these materials. In this work, we proposed a La3+/Al3+ codoping strategy in O3-Na(Ni1/3Mn1/3Fe1/3)O2 cathode materials and found that batteries with the Na (Ni1/3Mn1/3Fe1/3)0.998La0.001Al0.001O2 (NFM-La/Al) cathodes exhibited not only promoted capacity from 135.80 to 170.42 mAh g–1 at 0.2 C but also significantly enhanced cycling stability, with a 10% improvement in capacity retention compared with NFM cathodes after 300 cycles. Particularly, their rate performance was significantly improved as well. XRD and XPS tests indicated that La could expand the c-axis of NFM due to its larger ionic radius and thus significantly increased Na+ ion diffusion efficiency, and in addition, Al doping could effectively increase the content of Ni2+ and Mn4+ and thus greatly alleviated the negative Jahn–Teller effect caused by Mn3+. Moreover, consistent with XRD analyses, DFT calculations further substantiated the effectiveness of the La/Al codoping strategy by demonstrating the detailed atom substitution mechanism in the NFM crystal lattice. The boosted structure stability and Na+ diffusion kinetics may enhance the potential for practical applications of O3-type oxide cathodes.
LiNi0.8Co0.1Mn0.1O2 (NCM811) became a research hot point because of its low cost, environmental friendliness, and excellent electrochemical performance. However, Li+/Ni2+ intermixing is an essential factor affecting its applicability. Doping could be an important method to improve the electrochemical performance of NCM811-based cathode materials. In this work, La and Al co-doped NCM811 was prepared by a solid-state method. Results from X-ray diffraction (XRD), scanning electron microscopy (SEM), and energy-dispersive spectroscopy (EDS) and electrochemical performance were discussed in depth. These showed that when La and Al doping concentrations were 1 and 0.5%, the samples showed the best performance. The as-improved performances were mainly attributed to the reduced Li+/Ni2+ intermixing, suppressed phase transition, and decreased potential polarization and impedance.
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