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Improving cycling performance of the NaNiO2 cathode in sodium-ion batteries by titanium substitution
doi: 10.1088/2752-5724/ad5faa
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Abstract: AbstractO3-type layered oxide cathodes, such as NaNi0.5Mn0.5O2, have garnered significant attention due to their high theoretical specific capacity while using abundant and low-cost sodium as intercalation species. Unlike the lithium analog (LiNiO2), NaNiO2 (NNO) exhibits poor electrochemical performance resulting from structural instability and inferior Coulomb efficiency. To enhance its cyclability for practical application, NNO was modified by titanium substitution to yield the O3-type NaNi0.9Ti0.1O2 (NNTO), which was successfully synthesized for the first time via a solid-state reaction. The mechanism behind its superior performance in comparison to that of similar materials is examined in detail using a variety of characterization techniques. NNTO delivers a specific discharge capacity of ∼190 mAh g-1 and exhibits good reversibility, even in the presence of multiple phase transitions during cycling in a potential window of 2.0‒4.2 V vs. Na+/Na. This behavior can be attributed to the substituent, which helps maintain a larger interslab distance in the Na-deficient phases and to mitigate Jahn-Teller activity by reducing the average oxidation state of nickel. However, volume collapse at high potentials and irreversible lattice oxygen loss are still detrimental to the NNTO. Nevertheless, the performance can be further enhanced through coating and doping strategies. This not only positions NNTO as a promising next-generation cathode material, but also serves as inspiration for future research directions in the field of high-energy-density Na-ion batteries.
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Figure 1. Contour plot of in situ XRD data collected from the pre-heated NNTO mixture during calcination under O2 atmosphere.
Figure 3. (a)‒(e) Low- and high-magnification SEM images of NNTO prepared at different calcination temperatures. (f) Cycling performance of samples obtained at 700, 750, and 800 °C.
Figure 4. (a) STEM-EDS mapping of NNTO (800 °C). The random dots in the Ti map are artifacts. (b), (c) Low- and high-magnification cross-sectional HAADF STEM images of a FIB-prepared NNTO (800 °C) particle. (d) High-resolution image of the area indicated by the white dashed circle in (c).
Figure 5. (a) XRD patterns, (b), (c) SEM images, (d) primary particle size distributions, and (e) cycling performance of NNTO prepared with different molar Na/TM ratios.
Figure 6. (a) XRD patterns, (b), (c) SEM images, (d) primary particle size distributions, (e) first-cycle voltage profiles, and (f) cycling performance of NNTO prepared with different cooling rates.
Figure 7. (a) XRD patterns of NNTO prepared with different O2 flow rates of 1.4 l h-1 (cyan) and 7 l h-1 (purple). (b) SEM images at different magnifications of the 1.4 l h-1 sample.
Figure 8. (a) Long-term cycling performance of NNTO in coin half-cells and (b) corresponding rate capability.
Figure 9. Ex situ XANES spectra at the Ni K-edge of NNTO and NNO in the pristine and discharged states (after 10 cycles).
Figure 10. (a) 2D contour plot of operando XRD data collected during the first cycle at C/10 rate. (b) Illustration of crystal structures for O3, O’3, P3, O’’3, and O1. Cross-sectional SEM images of NNTO (c) in the pristine state and (d) after 200 cycles.
Figure 11. (a) Voltage profiles for the first five cycles (at C/30 rate followed by C/10 cycling) and corresponding cumulated hits. (b) Contour plot of acoustic activity (hit density) as a function of time and potential.
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