无机材料学报 ›› 2018, Vol. 33 ›› Issue (5): 475-482.DOI: 10.15541/jim20170330
所属专题: 离子电池材料
• 综述 • 下一篇
谭毅1,2, 薛冰1,2
收稿日期:
2017-07-06
修回日期:
2017-08-22
出版日期:
2018-05-20
网络出版日期:
2018-04-26
TAN Yi1,2, XUE Bing1,2
Received:
2017-07-06
Revised:
2017-08-22
Published:
2018-05-20
Online:
2018-04-26
摘要:
锂离子电池作为一种动力能源, 在电动汽车和各种储能系统中有着良好的应用前景。尖晶石结构的钛酸锂(Li4Ti5O12)负极材料具有较高的脱嵌锂电位平台、优异的循环稳定性、以及突出的安全性能, 被认为是一种非常有潜力的锂离子电池负极材料, 在锂离子动力电池中具有巨大的发展潜力。然而, 尖晶石型Li4Ti5O12存在着本征导电率低, 理论容量小等缺陷, 极大地限制了其规模化应用, 需要进一步改善和提高。本文总结了尖晶石型Li4Ti5O12材料在结构形貌、制备方法和性能方面的研究进展, 深入分析和讨论了离子掺杂、碳表面改性和纳米化等改性方法对尖晶石型Li4Ti5O12综合电化学性能的改善效果, 并展望了尖晶石型Li4Ti5O12作为锂离子电池负极材料未来的发展方向。
中图分类号:
谭毅, 薛冰. 锂离子电池负极材料钛酸锂的研究进展[J]. 无机材料学报, 2018, 33(5): 475-482.
TAN Yi, XUE Bing. Research Progress on Lithium Titanate as Anode Material in Lithium-ion Battery[J]. Journal of Inorganic Materials, 2018, 33(5): 475-482.
Ion | Radius /nm | Doping content molar ratio | Size/nm | Initial discharge capacity/(mAh.g-1) | Cycle performance/ (mAh.g-1) | Method | Ref. |
---|---|---|---|---|---|---|---|
Cation doping in the Li sites(radius 0.076 nm) | |||||||
Mg2+ | 0.0720 | 0.20 | 100-200 | 190.0(1C)a | 179.0(1C, 100)b; 150.0(5C, 100) | Solid state reaction | [30] |
Ca2+ | 0.1000 | 0.10 | 1000-2000 | 169.7(0.5C) | 162.4(1C, 100); 148.8(5C, 100) | Solid state reaction | [31] |
Sc3+ | 0.0745 | 0.05 | 200 | 174.0(1C); 94.0(40C) | 94.0(40C, 50) | Sol-Gel | [32] |
Cu2+ | 0.0730 | 0.05 | 200-600 | 158.0(0.1C) | 143.8(0.1C, 150) | Sol-Gel | [33] |
La3+ | 0.1032 | 0.06 | 24.5 | 169.0(0.1C) | 153.4(1C, 10); 146.9(5C, 10) | Liquid method | [34] |
Cation doping in the Ti sites (radiusTi3+0.067 nm, Ti4+0.0605 nm) | |||||||
Al3+ | 0.0535 | 0.15 | 50-200 | 216.0(1C); 163.0(10C) | 180.0(5C, 50); 160.0(10C, 50) | Cellulose-assisted glycine-nitratecombustion | [35] |
Zr4+ | 0.0720 | 0.03 | 200 | 165.0(5C); 152.0(10C) | 142.0(5C, 200); 127.0(10C, 200) | Liquid method | [36] |
Ce4+ | 0.0870 | 0.10 | <1000 | 190.0(0.2C); 40.0(2C) | 140.0(2C, 100) | Solid state reaction | [37] |
Ta5+ | 0.0640 | 0.05 | 500-1000 | 193.0(0.2C) | 132.0(5C, 100) | Solid state reaction | [38] |
Anions doping in the O site (radius 0.14 nm) | |||||||
Cl- | 0.181 | 0.2 | 3-8 μm | 148.7(0.5C) | 133.8(0.5C, 50) | Solid state reaction | [39] |
120.7(2C) | |||||||
Br- | 0.196 | 0.3 | 1-2 μm | 174.0(0.2C) | 138.0(10C, 100); 104.0(210C,100) | Solid state reaction | [40] |
表1 代表性阴阳离子掺杂Li4Ti5O12的Li, Ti, O各位点对性能的影响
Table 1 Summary of representative LTO doped with various cations/anions in the Li, Ti and O sites
Ion | Radius /nm | Doping content molar ratio | Size/nm | Initial discharge capacity/(mAh.g-1) | Cycle performance/ (mAh.g-1) | Method | Ref. |
---|---|---|---|---|---|---|---|
Cation doping in the Li sites(radius 0.076 nm) | |||||||
Mg2+ | 0.0720 | 0.20 | 100-200 | 190.0(1C)a | 179.0(1C, 100)b; 150.0(5C, 100) | Solid state reaction | [30] |
Ca2+ | 0.1000 | 0.10 | 1000-2000 | 169.7(0.5C) | 162.4(1C, 100); 148.8(5C, 100) | Solid state reaction | [31] |
Sc3+ | 0.0745 | 0.05 | 200 | 174.0(1C); 94.0(40C) | 94.0(40C, 50) | Sol-Gel | [32] |
Cu2+ | 0.0730 | 0.05 | 200-600 | 158.0(0.1C) | 143.8(0.1C, 150) | Sol-Gel | [33] |
La3+ | 0.1032 | 0.06 | 24.5 | 169.0(0.1C) | 153.4(1C, 10); 146.9(5C, 10) | Liquid method | [34] |
Cation doping in the Ti sites (radiusTi3+0.067 nm, Ti4+0.0605 nm) | |||||||
Al3+ | 0.0535 | 0.15 | 50-200 | 216.0(1C); 163.0(10C) | 180.0(5C, 50); 160.0(10C, 50) | Cellulose-assisted glycine-nitratecombustion | [35] |
Zr4+ | 0.0720 | 0.03 | 200 | 165.0(5C); 152.0(10C) | 142.0(5C, 200); 127.0(10C, 200) | Liquid method | [36] |
Ce4+ | 0.0870 | 0.10 | <1000 | 190.0(0.2C); 40.0(2C) | 140.0(2C, 100) | Solid state reaction | [37] |
Ta5+ | 0.0640 | 0.05 | 500-1000 | 193.0(0.2C) | 132.0(5C, 100) | Solid state reaction | [38] |
Anions doping in the O site (radius 0.14 nm) | |||||||
Cl- | 0.181 | 0.2 | 3-8 μm | 148.7(0.5C) | 133.8(0.5C, 50) | Solid state reaction | [39] |
120.7(2C) | |||||||
Br- | 0.196 | 0.3 | 1-2 μm | 174.0(0.2C) | 138.0(10C, 100); 104.0(210C,100) | Solid state reaction | [40] |
Ion | Radius/nm | Doping content molar ratio | Size/ nm | Initial discharge capacity/(mAh.g-1) | Cycle performance/ (mAh.g-1) | Method | Ref. |
---|---|---|---|---|---|---|---|
Zn2+ | 0.074 | 0.20 | 1000-2000 | (0-2.5 V) | 216.4(0.5C, 30) | Solid state reaction | [6] |
271.6(0.5C)a; 223.0(3C); | 198.0(3C, 100) | ||||||
186.0(5C, 200) | |||||||
206.0(5C) | |||||||
Nb5+ | 0.064 | 0.05 | (0-2.5 V) | 231.0(0.12C, 100) | Sol-Gel | [46] | |
351.0(0.12C) | |||||||
Ru4+ | 0.062 | 0.05 | 100-200 | (0.01-2.5 V) | 259.0(3C, 100); 131.0(60C, 100) | Reverse microemulsion method | [47] |
274.0(3C) | |||||||
Bi+3+ | 0.103 | 0.10 | 500-1000 | (0.01-2.5 V) | 203.0(1C, 50) | Solid state reaction | [48] |
214.0(1C) |
表2 低电位下代表性阳离子掺杂Li4Ti5O12的Li, Ti, O各位点对性能的影响
Table 2 Summary of representative LTO doped with various cations in the Li, Ti and O sites at low potential
Ion | Radius/nm | Doping content molar ratio | Size/ nm | Initial discharge capacity/(mAh.g-1) | Cycle performance/ (mAh.g-1) | Method | Ref. |
---|---|---|---|---|---|---|---|
Zn2+ | 0.074 | 0.20 | 1000-2000 | (0-2.5 V) | 216.4(0.5C, 30) | Solid state reaction | [6] |
271.6(0.5C)a; 223.0(3C); | 198.0(3C, 100) | ||||||
186.0(5C, 200) | |||||||
206.0(5C) | |||||||
Nb5+ | 0.064 | 0.05 | (0-2.5 V) | 231.0(0.12C, 100) | Sol-Gel | [46] | |
351.0(0.12C) | |||||||
Ru4+ | 0.062 | 0.05 | 100-200 | (0.01-2.5 V) | 259.0(3C, 100); 131.0(60C, 100) | Reverse microemulsion method | [47] |
274.0(3C) | |||||||
Bi+3+ | 0.103 | 0.10 | 500-1000 | (0.01-2.5 V) | 203.0(1C, 50) | Solid state reaction | [48] |
214.0(1C) |
Carbon source | Carbon content/wt% | Thickness/ nm | Initial discharge capacity/(mAh.g-1) | Cycle performance/ (mAh.g-1) | Method | Ref. |
---|---|---|---|---|---|---|
LPAN+CB | 3.64 | 3-5 | 166.2(10C) | 141.9(10C, 200) | Solid state reaction | [49] |
PEDOT | 10.00 | 10 | 168.7(1C) | 167.9(1C, 100) | Hydrothermal reaction | [50] |
Sucrose | 8.60 | 2-4 | 156.7(40C); 142.1(60C); 132.8(80C) | 114.2(40C, 200); 98.1(60C, 200) 82.7(80C, 200) | One-step liquid process | [51] |
Citric acid | 1.32 | 2-3 | 165.7(1C); 161.7(5C); 153.9(10C); 147.9(20C) | 144.9(20C, 50) | Sol-Gel | [52] |
Glucose | 8.96 | 8 | 170.9(0.5C) | 155.6(1C, 100) | Hydrothermal-solid state reaction | [53] |
表3 不同碳源、含量、厚度对碳包覆Li4Ti5O12的性能影响
Table 3 The effects of the carbon source, carbon content, thickness, and graphitization on the electrochemical performance of the carbon coated Li4Ti5O12
Carbon source | Carbon content/wt% | Thickness/ nm | Initial discharge capacity/(mAh.g-1) | Cycle performance/ (mAh.g-1) | Method | Ref. |
---|---|---|---|---|---|---|
LPAN+CB | 3.64 | 3-5 | 166.2(10C) | 141.9(10C, 200) | Solid state reaction | [49] |
PEDOT | 10.00 | 10 | 168.7(1C) | 167.9(1C, 100) | Hydrothermal reaction | [50] |
Sucrose | 8.60 | 2-4 | 156.7(40C); 142.1(60C); 132.8(80C) | 114.2(40C, 200); 98.1(60C, 200) 82.7(80C, 200) | One-step liquid process | [51] |
Citric acid | 1.32 | 2-3 | 165.7(1C); 161.7(5C); 153.9(10C); 147.9(20C) | 144.9(20C, 50) | Sol-Gel | [52] |
Glucose | 8.96 | 8 | 170.9(0.5C) | 155.6(1C, 100) | Hydrothermal-solid state reaction | [53] |
图5 Li4Ti5O12表面石墨烯层数的电子传导和锂离子传输过程示意图[57]
Fig. 5 Schematic illustration representing the electron conduction Li+ and Li+ transport according to the number of graphene layers on the LTO surface[57]
图6 Li4Ti5O12的TEM照片(a), Li4Ti5O12/C纳米棒的TEM照片(b, c)和HRTEM照片(d)[59]
Fig. 6 (a) TEM image of the Li4Ti5O12 nanoparticles and (b, c) TEM and (d) HRTEM images of Li4Ti5O12/C nanorods[59]
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