Phase transitions of Na-ion layered oxide materials and their influence on properties

Ding Fei-Xiang; Rong Xiao-Hui; Wang Hai-Bo; Yang Yang; Hu Zi-Lin; Dang Rong-Bin; Lu Ya-Xiang; Hu Yong-Sheng

doi:10.7498/aps.71.20220291

Abstract

Na-ion batteries possess great potential applications in the large-scale energy storage. The Na-ion layered oxide cathode (Na_xTMO₂) has received increasing attention in scientific and industrial research due to its high capacity, easy manufacture, adjustable voltage, and low cost. However, the larger the Na⁺ radius and the stronger the Na⁺-Na⁺ electrostatic repulsion is, which will lead to various structural configurations and complex structural transitions, resulting in multiple structure-property connections. In this paper, the structural types of Na-ion layered transition metal oxide cathode materials are introduced, and their structural evolutions during Na⁺ de/intercalation are summarized for revealing the mechanism for structural transformation of Na-ion layered transition-metal oxide cathode material and its effect on electrochemical performance; the existing challenges are discussed; the improvement strategies are proposed finally.

Keywords:

Authors and contacts

1.
Institute of Physics, Chinese Academy of Sciences, Beijing 100190, China
2.
College of Materials Science and Optoelectronic Technology, University of Chinese Academy of Sciences, Beijing 100049, China
3.
Huairou Division, Institute of Physics, Chinese Academy of Sciences, Beijing 101400, China

Corresponding author: Rong Xiao-Hui, rong@iphy.ac.cn ; Hu Yong-Sheng, yshu@iphy.ac.cn

Funds: Project supported by the National Natural Science Foundation of China (Grant Nos. 51725206, 52122214, 52072403), the Strategic Priority Research Program of the Chinese Academy of Sciences (Grant No. XDA21070500), Youth Innovation Promotion Association of the Chinese Academy of Sciences (Grant No. 2020006), the China Postdoctoral Science Foundation (Grant No. 2021M703460), and the Natural Science Foundation of Beijing, China (Grant No. 2212022).

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Cited By

图 1 (a)—(e)常见钠离子层状材料的晶体结构示意图, 插图为层状结构中过渡金属和钠离子多面体的连接机理示意图; (f)从垂直于过渡金属层的方向观察六方和单斜结构和晶胞参数的区别和联系

Figure 1. (a)–(e) Illustrations of crystal structures relevant to the Na⁺ layered oxide cathode materials, insets are the face-sharing schemes of TMO₆ and NaO₆ in the layered structures; (f) the view perpendicular to the layer direction highlighting the relationship between the hexagonal and monoclinic unit cells.

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图 2 各种3d过渡金属离子在钠离子电池层状氧化物中的特点^[13]

Figure 2. Comparison of the characteristics of 3d TM used in NIB layered cathode materials^[13].

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图 3 已报道的P2相和O3相中层状氧化物的阳离子势^[18]

Figure 3. Cationic potential of representative P2- and O3-type Na-ion layered oxides^[18].

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图 4 当碱金属阳离子和阴离子离子半径分别相同时O和P型配位环境中的阴离子距离对比^[19]

Figure 4. Comparison of anion-anion distances in O- and P-type coordinations assuming the same cation and anion radii^[19]

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图 5 (a) NaNi_0.5Mn_0.5O₂材料在2.2—3.8和2.2—4.5 V电压范围内的首周充放电曲线^[20]; (b) Na_1–xNi_0.5Mn_0.5O₂电极的非原位XRD图谱^[20], 星号代表集流体镍网的衍射峰; (c)NaNi_0.5Mn_0.5O₂材料首圈在C/20C倍率下充放电过程中的原位XRD图谱^[21]

Figure 5. (a) Initial charge-discharge curves of the NaNi_0.5Mn_0.5O₂ cell at a rate of 1/50C (4.8 mA/g) in the voltage ranges of 2.2–3.8 and 2.2–4.5 V versus sodium metal; (b) ex situ XRD patterns of the Na_1–xNi_0.5Mn_0.5O₂^[20], asterisks show a nickel mesh used as a current collector; (c) in situ XRD patterns of the NaNi_0.5Mn_0.5O₂ material at C/20 rate^[21].

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图 6 (a) Na_1–xNi_0.5Mn_0.5O₂电极的晶体结构转化示意图; (b) O3和O'3相之间的转化关系; (c) P3和P'3相之间的转化关系^[20]

Figure 6. (a) Schematic illustrations of the crystal structure of Na_1–xNi_0.5Mn_0.5O₂; (b) the transforming relationship between O3 and O'3; (c) the transforming relationship between between P3 and P'3^[20].

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图 7 (a) P3相过渡金属层可能的滑移方向α和β; (b) O1相的晶体结构示意图; (c)通过α和β滑移P3相向O3, O1, OPO₁3和O₁PO3相的转变示意图; (d)通过α和β滑移P3相向OO₁3, O₁OP3, POO₁3和PO₁O3相的转变示意图; (e)通过α和β滑移P3相向OP2相的转变示意图. 晶体结构观察方向为[100], 钠位为黄色多面体, 过渡金属位于紫色八面体, 结构示意图中没有考虑晶胞参数的变化^[19]

Figure 7. (a) P3 phase TM layer displacement vectors α and β; (b) schematic illustrations of the crystal structure of O1 phase; (c) phase transitions from P3 to O3, O1, OPO₁3 and O₁PO3 via shifting α and β; (d) phase transitions from P3 to OO₁3, O₁OP3, O₁OP3 and POO₁3 via shifting α or β; (e) phase transition from P3 to OP2 via shifting α and β. All structures viewed along [100] direction, all cell parameters changes have been ignored and TM octahedra are shown in purple and all Na sites in yellow^[19].

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图 8 (a) Na₂RuO₃的原位XRD图谱和充放电曲线; (b)根据原位实验确定的随钠含量变化的相图; (c)库仑力对Na_2–xRuO₃材料自有序过程的机理演示^[23]

Figure 8. (a) XRD patterns tested in situ during the first cycle of Na₂RuO₃ with the corresponding cycling curve; (b) phase diagram as determined from the in situ experiment as a function of the sodium content; (c) coulombic forces and resultant self-ordering in Na_2–xRuO₃^[23].

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图 9 (a) O3-NaFeO₂和(b) O3-NaCrO₂电极在不同充电截止电压的充放电曲线^[26,27]; (c)充电至高电压时Na_1–xCrO₂材料模拟和测试的XRD 图谱; (d) Na_xFeO₂材料在钠离子脱出过程的相图和铁迁移示意图^[28]; (e)脱钠过程中过渡金属离子迁移机理示意图^[29]

Figure 9. Charge-discharge curves of (a) NaFeO₂ and (b) NaCrO₂ cathode^[26,27]; (c) simulated and observed XRD patterns of Na_1–xCrO₂ cathode charged to high voltage; (d) scheme of phase evolution and iron migration upon sodium extraction in Na_xFeO₂^[28]; (e) a proposed mechanism of Meⁿ⁺ (Metal ion) migration process on the desodiated process^[29].

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图 10 充放电过程中O3型材料的结构演变汇总^[30]

Figure 10. Summary of structure evolution for O3-type materials during the charge-discharge process^[30].

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图 11 (a) P2-Na_2/3Ni_1/3Mn_2/3O₂的充放电曲线; (b) P2-Na_2/3Ni_1/3Mn_2/3O₂首周充电过程中的原位XRD图谱^[32]

Figure 11. (a) Charge-discharge curve of P2-Na_2/3Ni_1/3Mn_2/3O₂; (b) XRD patterns measured during the first charge of the P2-Na_2/3Ni_1/3Mn_2/3O₂ cathode in situ cell^[32].

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图 12 (a) P2-Na_2/3Ni_1/3Mn_2/3O₂的典型充电曲线; (b) P2-Na_δNi_1/3Mn_2/3O₂层内三棱柱位置钠离子/空位有序排布示意图(蓝色球代表占据Na_e位钠离子, 粉色球代表占据Na_f位钠离子)^[33]

Figure 12. (a) Typical charge profiles of P2-Na_2/3Ni_1/3Mn_2/3O₂; (b) in-plane Na⁺/vacancy orderings of P2-Na_δNi_1/3Mn_2/3O₂ in the triangular lattice (blue balls: Na-ions on Na_e sites, pink balls: Na-ions on Na_f sites) ^[33].

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图 13 (a) P2-Na_2/3Ni_1/3Mn_2/3O₂和(b) P2-Na_2/3Ni_1/3Mn_1/3Ti_1/3O₂电极在2.5—4.3 V电压范围内首周充电过程中的原位XRD图谱^[34]

Figure 13. In situ XRD patterns of (a) P2-Na_2/3Ni_1/3Mn_2/3O₂ and (b) P2-Na_2/3Ni_1/3Mn_1/3Ti_1/3O₂ electrodes during the first charge between 2.5 and 4.3 V^[34].

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图 14 P2-Na_2/3Ni_1/3Mn_2/3O₂电极在1.5—4.0 V电压范围内的首周充放电曲线^[35]

Figure 14. Initial charge-discharge curves of P2-Na_2/3Ni_1/3Mn_2/3O₂ in the voltage of 1.5–4.0 V^[35].

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图 15 (a) P2相过渡金属层可能滑移的方向γ; (b)通过γ滑移P2相向O2相的转变示意图; (c)通过γ滑移P2相向OP4相的转变示意图. 晶体结构观察方向为[100], 钠位为黄色多面体, 过渡金属位于紫色八面体, 结构示意图中没有考虑晶胞参数的变化^[19]

Figure 15. (a) P2 phase TM layer displacement vectors γ; (b) phase transitions from P2 to O2 via shifting γ; (c) phase transitions from P2 o OP4 via shifting γ. All structures viewed along [100] direction, all cell parameters changes have been ignored and TM octahedra are shown in purple and all Na sites in yellow^[19].

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图 16 (a) (b) P2-和P3-Na_0.6Li_0.2Mn_0.8O₂正极材料钠离子脱嵌过程中的拓扑保护机制^[40]

Figure 16. (a)(b) Topological protection mechanism during Na-ion deintercalation of P2-and P3-Na_0.6Li_0.2Mn_0.8O₂^[40].

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图 17 充放电过程中P2型材料的结构演变汇总^[30]

Figure 17. Summary of structure evolution for P2-type materials during the charge-discharge process^[30].

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图 18 (a) Na_0.66Li_0.22Ti_0.78O₂电极在0.1 C倍率下0.4—2.5 V电压范围内的充放电曲线; (b) Na_0.66Li_0.22Ti_0.78O₂电极在C/7倍率下首周充放电过程中的原位XRD图谱^[41]; (c) Na_0.6Cr_0.6Ti_0.4O₂电极在0.1 C倍率下0.5—2.5 V电压范围内的首周充放电曲线^[42]; (d) Na_0.6Cr_0.6Ti_0.4O₂电极在C/5倍率下首周充放电过程中的原位XRD图谱^[42]

Figure 18. (a) The discharge-charge curves of Na_0.66Li_0.22Ti_0.78O₂ at a current rate of 0.1 C (10.6 mA/g) in the voltage range of 0.4–2.5 V; (b) in situ XRD patterns collected during the first discharge-charge of the Na_0.66Li_0.22Ti_0.78O₂ electrode under a current rate of C/7^[41]; (c) the first discharge-charge curve of Na_0.6Cr_0.6Ti_0.4O₂ in the voltage range of 0.5–2.5 V; (d) in situ XRD patterns collected during the first discharge-charge of the Na_0.6Cr_0.6Ti_0.4O₂ electrode under a current rate of C/5^[42]_.

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图 19 O3-Na_x[Ni_0.33Fe_0.33Mn_0.33]O₂在(a) 2.0—4.0 V和(b) 2.0—4.3 V之间同步辐射原位XRD测试结果以及充放电曲线^[57]

Figure 19. In situ XRD patterns tested during cycling of Na_xNi_1/3Fe_1/3Mn_1/3O₂ electrode in the voltage range of (a) 2.0–4.0 V and (b) 2.0–4.3 V^[57].

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图 20 (a) NaNi_0.5Mn_0.4Ti_0.1O₂和(b) NaNi_0.4Cu_0.1Mn_0.4Ti_0.1O₂电极在2.0—4.5 V电压范围内的原位XRD图谱^[63]

Figure 20. In situ XRD patterns of (a) NaNi_0.5Mn_0.4Ti_0.1O₂ and (b) NaNi_0.4Cu_0.1Mn_0.4Ti_0.1O₂ electrode in the voltage range of 2.0–4.5 V^[63]

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图 21 (a)高熵构型稳定O3结构的机理阐释^[68]; (b) NaNi_0.6Fe_0.25Mn_0.15O₂材料在2.0—4.2 V电压范围内的原位XRD图谱和(c)结构演变示意图^[69]

Figure 21. (a) Possible mechanism of high-entropy composition in facilitating layered O3-type structure^[68]; in situ XRD patterns of (b) NaNi_0.6Fe_0.25Mn_0.15O₂ electrode in the voltage range of 2.0–4.2 V and (c) schematic of structural evolution^[69].

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图 22 (a)P2-和(c)O3-Na_2/3Fe_2/3Mn_1/3O₂ 样品的XRD 谱和SEM图片;(b) P2-和(d)O3- Na_2/3Fe_2/3Mn_1/3O₂ 样品前两周在1.5—4.2 V电压范围内的充放电曲线对比^[71]

Figure 22. XRD patterns and SEM images of (a) P2- and (c) O3- Na_2/3Fe_2/3Mn_1/3O₂ samples; comparison of charge-discharge capacity of (b) P2- and (d) O3- Na_2/3Fe_2/3Mn_1/3O₂ within the 1 st and 2 nd cycles in the voltage range of 1.5–4.2 V^[71].

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图 23 不同冷却方式对材料晶体结构中空位的影响示意图^[74]

Figure 23. Schematic illustration of the effects of different cooling methods on the vacancies of the crystal structures^[74].

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表 1 常见的结构对应的空间群和原子坐标

Table 1. The space groups and corresponding atomic positions of reported structures.

结构	空间群 (代号)	原子占位
结构		Na_e	Na_f	Na	M	O
O3	${R}\bar{3}{m}$ (167)	—	—	3b (0, 0, 1/2)	3a (0, 0, 0)	6c (0, 0, ~0.27)
O'3	C2/m (12)	—	—	2d (0, 1/2, 1/2)	2a (0, 0, 0)	4i (~0.28, 0, ~0.8)
P3	R3m (160)	—	—	3a (0, 0, ~0.17)	3a (0, 0, 0)	3a (0, 0, ~0.4)
P2	P6₃/mmc (194)	2d (2/3, 1/3, 1/4)	2b (0, 0, 1/4)	—	2a (0, 0, 0)	4f (1/3, 2/3, ~0.09)
O2	P6₃mc (186)	—	—	2b (1/3, 2/3, ~0.24)	2b (2/3, 1/3, 0)	2b (2/3, 1/3, ~0.39)

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