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化学进展 2022, Vol. 34 Issue (4): 857-869 DOI: 10.7536/PC210441 前一篇   后一篇

• 综述 •

掺杂对钠离子电池正极材料性能影响机制的研究

李婧婧, 李洪基, 黄强, 陈哲*()   

  1. 华北电力大学 北京 102206
  • 收稿日期:2021-04-22 修回日期:2021-08-06 出版日期:2022-04-24 发布日期:2021-12-02
  • 通讯作者: 陈哲
  • 基金资助:
    国家电网公司科技项目(5419-201999542A-0-0-00)
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Study on the Mechanism of the Influence of Doping on the Properties of Cathode Materials of Sodium Ion Batteries

Jingjing Li, Hongji Li, Qiang Huang, Zhe Chen()   

  1. North China Electric Power University,Beijing 102206, China
  • Received:2021-04-22 Revised:2021-08-06 Online:2022-04-24 Published:2021-12-02
  • Contact: Zhe Chen

钠元素在地壳中的丰度是锂元素的1000倍,资源丰富,价格低廉。同时,钠离子电池负极可采用廉价的铝箔替代铜箔,且低温特性更加优异,在能量型、备用型储能场景均具有较好应用前景,因而钠离子电池被认为是下一代大规模储能技术的理想选择之一。然而,相对锂离子而言,钠离子较大的离子半径和质量极大限制了其在电极材料中的可逆脱嵌,导致电池的工作电压和能量密度相对较低。在钠离子电池材料体系中,正极材料的研究尤为需要长足的进步。本文对现有的典型钠离子电池正极材料进行了综述,包括层状金属氧化物、聚阴离子化合物和普鲁士蓝类化合物,并重点分析了掺杂对钠离子电池正极材料性能的影响。通过元素掺杂可提高材料的循环可逆性、增加其可逆容量、提升钠离子扩散动力学性能,能够在一定程度上改变晶格的性质,增强晶格稳定性、电子导电性、钠离子嵌脱动力学性能等。本文总结了掺杂应用在现有材料中获得的成果,并对正极材料未来的研究方向以及发展前景提出了展望。

关键词： 钠离子电池, 正极材料, 掺杂

The abundance of sodium salt in the earth’s crust is 1000 times higher than that of lithium. At the same time, low-cost aluminum foil can be used as the anode of sodium ion battery instead of copper foil, and the low-temperature characteristics are more excellent, which has a good application prospect in energy storage and standby energy storage scenarios. Therefore, sodium ion battery is considered one of the ideal choices for the next generation of large-scale energy storage technology. However, compared with lithium ion, the large ion radius and mass of sodium ion greatly limit its reversible deintercalation in electrode materials, resulting in relatively low working voltage and energy density of the battery. In the sodium ion battery materials system, the research of cathode materials needs great progress. In this paper, the existing typical cathode materials for sodium ion batteries are reviewed, including layered metal oxides, polyanions and Prussian blue compounds. The effect of doping on the performance of cathode materials for sodium ion batteries is analyzed. The cycling reversibility, reversible capacity and diffusion kinetics of sodium ions can be improved by element doping, which can change the properties of the crystal lattice to a certain extent, and enhance the stability, electronic conductivity and intercalation kinetics of sodium ions. In this paper, the achievements of doping application in the existing materials are summarized, and the future research direction and development prospect of cathode materials are put forward.

Contents

1 Research background

2 Doping modification of cathode materials for sodium ion batteries

2.1 Modification of layered metal oxides by doping

2.2 Modification of Prussian Blue by doping

2.3 Modification of polyanionic compounds by doping

3 Doping modification principle of cathode materials for sodium ion batteries

3.1 Restrain phase transition and stabilize structure

3.2 Increase the layer spacing and improve the dynamics

3.3 Improving the discharge capacity of cathode materials

3.4 Improve the electronic conductivity and ionic conductivity of materials

3.5 Inhibition of Na+ Vacancy ordered structure

4 Conclusion and outlook

Key words: sodium ion battery, positive material, doping
()
表1 掺杂在钠离子电池正极材料中的应用
Table 1 Application of doping in cathode material of sodium ion battery
Type Cathode material Voltage Capacity
(mAh/g)		 Cycle performance Doping method ref
Layered
metal
oxide		 NaxMn0.9Co0.1O2 1.5~3.8 V 165(50 mA/g) 75% (After100 cycle) Combustion synthesis 29
NaxFe1/2Mn1/2O2 1.5~4.3 V 190(0.05 C) 79% (After 30 cycle) Solid-state reaction 30
NaxMn2/3Ni1/3O2 2.3~4.5 V 134(1.7 mA/g ) 64% (After 10 cycle) Co-precipitation technique 31
Na0.5Mn0.48Co0.5Al0.02O2 1.5~4.3 V 134 (85 mA/g ) 83% (After 100 cycle) Sol-gel method 32
Na0.9[Cu0.22Fe0.30Mn0.48]O2 2.5~4.05 V 100(0.1 C) 97% (After 100 cycle) Solid-state reaction 33
NaCr1/3Fe1/3Mn1/3O2 1.5~4.2 V 186(0.05 C) 54% (After 35 cycle) Solid-state reaction 34
Na0.67Mn0.67Ni0.28Mg0.05O2 2.5~4.35 V 123(0.1 C) 85% (After 50 cycle) Sol-gel method 35
Prussian blue NayFe0.4Mn0.1[Fe(CN)6] 2.0~4.2 V 119(1 C) 65% (After 350 cycle) Ball-milling method 36
NaxNi0.3Fey[Fe(CN)6] 2.0~4.0 V 117(10 mA/g) 86.3% (After 90 cycle) Co-precipitation technique 37
Na2Mn0.15Co0.15Ni0.1Fe0.6Fe(CN)6 2.0~4.0 V 111(1 C) 78.7% (After 1500 cycle) Co-precipitation technique 38
Na1.76Ni0.12Mn0.88
[Fe(CN)6]0.98		 2.0~4.0 V 118(10 mA/g) 83.8% (After 800 cycle) Co-precipitation technique 39
Na2Ni0.4Co0.6Fe(CN)6 2.0~4.2 V 92(50 mA/g) 89.5% (After 100 cycle) Co-precipitation technique 40
Na2CoFe(CN)6 2.0~4.1 V 150(10 mA/g) 90% (After 200 cycle) Citrate-assisted controlled crystallization method 41
Na0.39Fe0.77Ni0.23
[Fe(CN)6]0.79·3.45H2O		 2.0~4.0 V 106(10 mA/g) 96% (After 100 cycle) Co-precipitation technique 42
Polyanionic
compounds		 NaFePO4@C 1.5~4.5 V 145(0.2 C) 89% (After 6300 cycle) Electrospinning technique 43
Br/N/a-C@Na3V2(PO4)3 2.5~4.3 V 83(0.1 C) 80% (After 500 cycle) Sol-gel assisted
hydrothermal		 44
Na3Mn1.6Fe0.4P3O11@C 1.8~4.3 V 84.9(0.1 C) 74% (After 100 cycle) Citric based sol-gel method and carbothermal reduction methods 45
Na3V1.9Co0.1(PO4)2F3 1.6~4.6 V 111.3(0.1 C) 70% (After 80 cycle) Sol-gel method 46
Na3MnTi(PO4)3/C 1.5~4.2 V 160(0.2 C) 92% (After 500 cycle) Spray-drying method 47
Na4MnCr(PO4)3 1.4~4.6 V 160.5(0.05 C) 74% (After 50 cycle) Sol-gel method 48
Na4Mn3(PO4)2(P2O7) 1.7~4.5 V 121(0.05 C) 86% (After 100 cycle) Solid-state reaction 49
图1 层状金属氧化物结构示意图及相变过程[8]
Fig. 1 Structure diagram and phase transition process of layered metal oxides[8]. Copyright 2014, American Chemical Society
图2 (a) Na0.9[Cu0.22Fe0.30Mn0.48]O2电极的第一和第二恒流充放电曲线在2.5~4.05 V之间以0.1 C (10 mA/g)的速率循环;(b) 在0.1 C速率下的容量、库仑效率和能量转换效率与循环次数的关系;(c) 倍率性能[33]
Fig. 2 (a) The first and second constant current charge discharge curves of Na0.9[Cu0.22Fe0.30Mn0.48]O2 electrode were cycled between 2.5~4.05 V at the rate of 0.1 C (10 mA/g); (b) the relationship between the capacity, coulomb efficiency and energy conversion efficiency at the rate of 0.1 C and the number of cycles; (c) the rate performance[33]. Copyright 2015, John Wiley and Sons
图3 (a) 各种P2型Na0.67Mn0.67Ni0.33-xMgxO2电极(x = 0,0.02,0.05,0.10和0.15)在0.1 C下的恒流充放电电压分布;(b) 各种P2型Na0.67Mn0.67Ni0.33-xMgxO2电极(x = 0,0.02,0.05,0.10,0.15)在50个循环中的循环性能;(c) P2型Na0.67Mn0.67Ni0.33-xMgxO2电极(x = 0.10和0.15)在100圈中的循环性能[35]
Fig. 3 (a) Constant current charge discharge voltage distribution of various P2 type Na0.67Mn0.67Ni0.33-xMgxO2 electrodes (x = 0, 0.02, 0.05, 0.10 and 0.15) at 0.1 C;(b) cycling performance of various P2 type Na0.67Mn0.67Ni0.33-xMgxO2 electrodes (x = 0, 0.02, 0.05, 0.10 and 0.15) in 50 cycles;(c) cycling performance of P2 type Na0.67Mn0.67Ni0.33-xMgxO2 electrodes (x = 0.10 and 0.15) in 100 cycles[35]. Copyright 2016, John Wiley and Sons
图4 (a) NaCr1/3Fe1/3Mn1/3O2在0.03 C (5 mA/g)电流下的恒流循环曲线与Na+/Na的关系;(b) 在1.5~4.2 V的电位范围内,NaCr1/3Fe1/3Mn1/3O2电极在0.05 C (10 mA/g)下的恒流循环曲线与Na+/Na的关系;(c) NaCr1/3Fe1/3Mn1/3O2电极在1.5~4.1 V之间循环的前三圈循环伏安曲线[34]
Fig. 4 (a) The relationship between the constant current cyclic curve and Na+/Na of NaCr1/3Fe1/3Mn1/3O2 electrode at 0.03 C (5 mA/g); (b) the relationship between the constant current cyclic curve and Na+/Na of NaCr1/3Fe1/3Mn1/3O2 electrode at 0.05 C (10 mA/g) in the potential range of 1.5~4.2 V; (c) The first three cycles of cyclic voltammetry of NaCr1/3Fe1/3Mn1/3O2 electrode between 1.5~4.1 V[34]. Copyright 2017, The Royal Society of Chemistry
图5 普鲁士蓝类似物的结构[62]
Fig. 5 Structure of Prussian blue analogues[62]. Copyright 2012, The Royal Society of Chemistry
图6 (a) 电流密度为10 mA/g时,NixFe-PBAs的恒流曲线;(b) NixFe-PBAs扫描速率为0.1 mV/s时的循环伏安曲线[37]
Fig. 6 (a) Constant current curve of NixFe-PBAs at current density of 10 mA/g; (b) cyclic voltammetry curve of NixFe-PBAs at scanning rate of 0.1 mV/s[37]. Copyright 2017, The Royal Society of Chemistry
图7 (a) PBM、PBN和PBMN的恒流充放电特性; (b) PBM、PBN和PBMN的循环性能[39]
Fig. 7 (a) The galvanostatic charge-discharge profiles of PBM, PBN and PBMN; (b) cyclic performances of PBM, PBN and PBMN[39]. Copyright 2014, The Royal Society of Chemistry
图8 NaFePO4@C正极材料的倍率性能[43]
Fig. 8 NaFePO4@C rate performance of cathode materials[43]. Copyright 2018, John Wiley and Sons
图9 (a,b) Br/N/a-C@NVP-1,Br/N/a-C@NVP-2,Br/N/a-C@NVP-3,纯NVP和NVP/C正极的倍率性能[44]
Fig. 9 (a, b) Rate performance of Br/N/a-C@NVP-1, Br/N/a-C@NVP-2, Br/N/a-C@NVP-3, pure NVP and NVP/C cathode[44]. Copyright 2020, The Royal Society of Chemistry
图10 (a) Na3V2-xMgx(PO4)3/C在不同电流密度下的倍率性能; (b) Na3V2-xMgx(PO4)3/C在10 C下的循环性能; (c) Na3V2-xMgx(PO4)3/C在20 C下的循环性能[86]
Fig. 10 (a) Rate capability of Na3V2-xMgx(PO4)3/C at different current densities; (b) cycling stability of Na3V2-xMgx(PO4)3/C at 10 C; (c) cycling stability of Na3V2-xMgx(PO4)3/C at 20 C[86]. Copyright 2015, The Royal Society of Chemistry
图11 Na0.66Ni0.33Mn0.67O2掺杂材料在相结构转变的原理示意图[87]
Fig. 11 Schematic diagram of the phase structure transformation of Na0.66Ni0.33Mn0.67O2 doped materials[87]. Copyright 2016, American Chemical Society
表2 三种正极材料的导电性
Table 2 Conductivity of three cathode materials
Sample Resistance (Ω·m) Conductivity(S·m-1)
Pure ZrO2 4.81 × 106 2.08 × 10-7
Na0.75Mn0.55Ni0.25Co0.05Fe0.15O2 3.21 × 105 3.12 × 10-6
Na0.75Mn0.55Ni0.25Co0.05Fe0.10Zr0.05O2 1.92 × 105 5.20 × 10-6
图12 (a) 模拟800 K温度下P2-Na0.57NMT中Na+的运动轨迹; (b) Na+扩散系数Arrhenius图[92]
Fig. 12 (a) Trajectories of Na+ in P2-Na0.57NMT simulated at a temperature of 800 K; (b) Arrhenius plot of Na+ diffusion coefficients[92]. Copyright 2018, American Association for the Advancement of Science
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