Abstract
Cation-disordered oxide materials working as cathodes for Li-ion batteries have been at a standstill because of their structurally limited specific capacities (below 175 mAh g-1 in most cases). In this work, we have introduced 4d0 Nb5+ into host material LiNi0.5Ti0.5O2 to synthesize Ni-based cation-disordered Fm3̅m Li-Ni-Ti-Nb-O compounds of Li1+x/100Ni1/2-x/100Ti1/2-x/100Nbx/100O2 (x = 0, 5, 10, 15, 20) through a sol-gel method, showing particle sizes of less than 200 nm. Taking Li1.2Ni0.3Ti0.3Nb0.2O2 with the best performance (an average voltage of ∼2.7 V and high discharge capacity of 221.5 mAh g-1) among oxides as a model, we study the relationship between the structure, morphology, redox mechanism, and electrochemical performance of cation-disordered oxides through a combination of X-ray diffraction (XRD), scanning electron microscopy, transmission electron microscopy, X-ray photoelectron spectroscopy, and X-ray absorption near-edge spectroscopy tests and in situ XRD with electrochemistry. The obtained results indicate that the improved capacity is mainly ascribed to Nb5+, which optimizes the Ni2+/Ni4+ practical capacity and effectively stabilizes the O2-/O- redox reaction. The results emphasize that Li-Ni-Ti-Nb-O compounds are promising members in the family of cation-disordered transition-metal oxide materials.
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