钠离子层状氧化物材料相变及其对性能的影响

丁飞翔; 容晓晖; 王海波; 杨佯; 胡紫霖; 党荣彬; 陆雅翔; 胡勇胜

doi:10.7498/aps.71.20220291

摘要

钠离子电池近年来在大规模储能领域展现出优异的发展和应用前景. 由于钠离子层状过渡金属氧化物正极材料(Na_xTMO₂)具有比容量高、容易制备、电压可调和成本低的优势, 在学术界和产业界得到了广泛的关注与研究. 但较大的Na⁺半径和较强的Na⁺-Na⁺静电排斥作用, 导致Na_xTMO₂具有多种结构类型和复杂的结构转变, 以及由此形成了多重结构-性能关系. 本文详细介绍了Na_xTMO₂的结构类型, 综述了在Na⁺脱出/嵌入过程中引发的结构演变, 旨在揭示钠离子层状过渡金属氧化物正极材料结构转变机理及其对电化学性能的影响, 最后讨论了现存的挑战并提出了改进策略.

关键词:

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:

作者及机构信息

1.
中国科学院物理研究所, 北京　100190

2.
中国科学院大学, 材料科学与光电技术学院, 北京　100049

3.
中国科学院物理研究所, 怀柔研究部, 北京　101400

通信作者: 容晓晖, rong@iphy.ac.cn ; 胡勇胜, yshu@iphy.ac.cn

作者简介:

容晓晖, 中国科学院物理研究所特聘研究员、博士生导师. 主要从事新型钠离子电池正极材料(层状氧化物、磷酸盐、普鲁士蓝等)、固态钠电池(NASICON固体电解质、新型聚合物固体电解质的设计与合成)研究. 至今已在Nature Sustainability、Joule、Journal of American Chemical Society、Energy Storage Materials等国际知名学术期刊上发表学术论文30余篇, 申请20余项国际和中国发明专利, 参与撰写《钠离子电池科学与技术》, 撰写原创科普文章50余篇. 目前担任ACS Energy Letters等多个专业杂志的审稿人

胡勇胜, 中科院物理研究所研究员, 英国皇家化学学会会士/英国物理学会会士, 中国科协十大代表. 先后承担了国家科技部863创新团队、国家杰出青年科学基金等项目. 自2001年以来, 主要从事先进二次电池的应用基础研究, 立足科学前沿和聚焦国家重大需求, 注重基础与应用, 在钠(锂)离子电池正负极材料、多尺度结构演化、功能电解质材料等方面取得多项创新性研究结果. 在Science、Nature Energy、Nature Mater.、Joule、Nature Commun.、Science Adv.等国际重要学术期刊上共合作发表论文200余篇, 引用30000余次, H-因子94, 连续8年入选科睿唯安 “高被引科学家”名录. 合作申请60余项中国发明专利、已授权40项专利(包括多项美国、日本、欧盟专利). 目前担任ACS Energy Letters杂志资深编辑. 最近所获荣誉与奖励包括第十四届中国青年科技奖、国际电化学学会Tajima Prize、英国皇家学会牛顿高级访问学者等. 开发的钠离子电池技术在第三届国际储能创新大赛中荣获“2019储能技术创新典范TOP10”和“评委会大奖”、第九届中国科学院北京分院科技成果转化特等奖、2020年科创中国·科技创新创业大赛TOP10、2020年中关村国际前沿科技创新大赛总决赛亚军、入选2020年度中国科学十大进展30项候选成果, 合著《钠离子电池科学与技术》专著一本(科学出版社2020年出版)

基金项目: 国家自然科学基金(批准号: 51725206, 52122214, 52072403)、中国科学院战略性先导科技专项(批准号: XDA21070500)、中国科学院青年创新促进会(批准号: 2020006)、中国博士后科学基金(批准号: 2021M703460)和北京市自然科学基金(批准号: 2212022)资助的课题.

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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施引文献

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

Fig. 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]

Fig. 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]

Fig. 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]

Fig. 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]

Fig. 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]

Fig. 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]

Fig. 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]

Fig. 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]

Fig. 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]

Fig. 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]

Fig. 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]

Fig. 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]

Fig. 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]

Fig. 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]

Fig. 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]

Fig. 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]

Fig. 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]

Fig. 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]

Fig. 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]

Fig. 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]

Fig. 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]

Fig. 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]

Fig. 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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