Layered oxide cathode materials based on molecular orbital hybridization for high voltage sodium-ion batteries

doi:10.19799/j.cnki.2095-4239.2021.0496

Abstract

Abstract:

O3-type sodium-layered transition-metal oxides, NaNi_0.5Mn_0.5O₂, are one of the most promising cathode materials. However, the application of O3-NaNi_0.5Mn_0.5O₂ cathode material is limited due to the transition metal layer's slip during charge and discharge processes, with multiple irreversible complex phase transitions. In addition, its energy density is limited due to the capacity of O3-NaNi_0.5Mn_0.5O₂ electrode, which is mainly concentrated in the low-voltage region around 3 V, and O3-P3 phase transition easily occurred in this region. This study proposes a precise chemical element substitution strategy for successfully solving these problems Doping with Sn⁴⁺ inhibits the transition metal layer's slip and the irreversible multiphase transformation. Meanwhile, Sn⁴⁺ cannot be hybridized with the O 2p orbital due to the unique outer electronic structure, which lacks a single electron in its d orbital. The O 2p orbital only hybridized with the Ni e_g orbital, increasing the ionic degree of Ni—O bond and Ni's redox potential. Therefore, O3-NaNi_0.5Mn_0.5O₂ can display a high midpoint voltage of 3.28 V. Meanwhile, the electrode material exhibits excellent electrochemical performance and kinetic properties. The controllable redox potential of O3-type cathode material was realized based on molecular orbital hybridization theory to obtain the high-voltage layered oxide cathode materials sodium-ion batteries.

Key words: sodium-ion battery, layered cathode material, molecular orbital hybridization, high voltage, phase transformation mechanism

CLC Number:

TM 911.14

Haiyan HU, Shulei CHOU, Yao XIAO. Layered oxide cathode materials based on molecular orbital hybridization for high voltage sodium-ion batteries[J]. Energy Storage Science and Technology, 2022, 11(4): 1093-1102.

Figures/Tables 8

Fig. 1

Fig. 2

Table 1

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Fig. 5

Table 2

Table 3

References 69

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理论化学式	实际测量原子比
理论化学式	Na	Ni	Sn
NaNi_0.5Sn_0.5O₂	0.996	0.502	0.497

正极材料组成	合成方法	中值电压/V	参考文献
NaNi_0.5Sn_0.5O₂	固相法	3.28	本文
Na_0.66Li_0.18Mn_0.71Ni_0.21Co_0.08O₂₊_δ	共沉淀法+固相法	3.2	[40]
Na_0.44Co_0.1Mn_0.9O₂	热聚合法	约2.667	[61]
Na[Mn_0.25Fe_0.25Co_0.25Ni_0.25]O₂	固相法	3.21	[62]
Na_0.9Ni_0.45Mn_0.55O₂	溶胶凝胶法	3.03	[63]
Na_0.5[Li_0.2Fe_0.4Mn_0.4]O₂	溶胶凝胶法	2.85	[64]
Na_0.67Mn_0.97Mo_0.03O₂	固相法	2.61	[65]
Na₄FeV(PO₄)₃	溶胶凝胶法	3.13	[66]
Na₃Fe₂(PO₄)(P₂O₇)	喷雾干燥法	3.1	[67]
NaFe_0.45Co_0.5Mg_0.05O₂	固相法	3.1	[68]
Na_0.9Cu_0.22Fe_0.30Mn_0.48O₂	固相法	3.2	[69]

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