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化学进展 2019, Vol. 31 Issue (8): 1166-1176 DOI: 10.7536/PC190140 前一篇   后一篇

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过渡金属硫化物改性锂硫电池正极材料

樊潮江, 燕映霖**(), 陈利萍, 陈世煜, 蔺佳明, 杨蓉   

  1. 西安理工大学化学电源研究所 西安 710048
  • 收稿日期:2019-01-30 出版日期:2019-08-15 发布日期:2019-05-30
  • 通讯作者: 燕映霖
  • 基金资助:
    国家国际科技合作专项(2015DFR50350); 和国家自然科学基金项目(51702256)
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Transition-Metal Sulfides Modified Cathode of Li-S Batteries

Chaojiang Fan, Yinglin Yan**(), Liping Chen, Shiyu Chen, Jiaming Lin, Rong Yang   

  1. Chemical Power Research Institute, Xi’an University of Technology, Xi’an 710048, China
  • Received:2019-01-30 Online:2019-08-15 Published:2019-05-30
  • Contact: Yinglin Yan
  • About author:
    ** E-mail:
  • Supported by:
    International Science and Technology Cooperation Program of China(2015DFR50350); National Natural Science Foundation of China(51702256)

锂硫电池(LSBs)由于单质硫正极具有超高能量密度(2600 Wh/kg)和超高理论比容量(1675 mAh/g),且环境友好、成本低廉,被认为是最有前景的储能体系之一。然而,硫正极的绝缘性和严重体积膨胀以及多硫化物(LiPSs)的“穿梭效应”等问题导致活性物质利用率低、循环稳定性差及电化学反应动力不足,严重阻碍了LSBs的商业化发展。最新研究表明,过渡金属硫化物作为载体或添加剂能够显著改善LSBs正极材料的电化学性能。本文从等效/共正极作用、导电性增强作用、LiPSs吸附作用和电化学反应催化作用四个方面梳理了过渡金属硫化物在LSBs正极材料中的改性机理,并指出多元过渡金属硫化物复合﹑纳米结晶和量子化作为增加比表面积和活性位点的方法是过渡金属硫化物用于锂硫电池正极材料的重要发展方向,可大幅提升LSBs的电化学性能。

关键词： 锂硫电池, 过渡金属硫化物, 电化学性能, 穿梭效应, 吸附作用, 催化作用

Lithium-sulfur batteries(LSBs) are considered as one of the most promising energy storage systems due to the ultra-high theoretical energy density(2600 Wh/kg) and ultra-high theoretical specific capacity(1675 mAh/g), environmental friendliness and low-cost of sulfur cathode. However, the insulation of sulfur cathode, the volumetric strain and the “shuttle effect” of polysulfides lead to problems such as low utilization rate of active materials, poor cycle stability and low redox kinetics, which seriously hinder the commercial development of LSBs. Recent studies have shown that transition metal sulfides as host or additives can significantly improve the electrochemical performance of LSBs cathode materials. In this paper, the modification mechanism of transition metal sulfides in LSBs cathode materials is reviewed from four aspects: equivalent/common positive electrode effect, conductivity enhancement, LiPSs adsorption and electrochemical reaction catalysis. It is pointed out that multi-transition metal sulfides composite, nano-crystallization and quantization as important areas for increasing the specific surface area and active sites should be used as transition metal sulfides for lithium-sulfur battery cathode materials, which can greatly improving the electrochemical performance of LSBs.

Key words: lithium sulfur batteries, transition-metal sulfides, electrochemical performance, shuttle effect, adsorption, catalysis
()
图1 过渡金属硫化物用于LSBs促进作用示意图
Fig. 1 Schematic diagram of the effect of transition metal sulfides on the promotion of LSBs
图2 MoSx作为LSBs硫等效材料的电化学性能:(a)MoS2等效正极充放电曲线,(b)“激活”后MoS2等效正极充放电曲线,(c,d) MoS3等效正极电化学性能曲线[34]
Fig. 2 Electrochemical performance of MoSx as a sulfur equivalent material for LSBs:(a)MoS2 equivalent positive charge and discharge curve,(b)MoS2 equivalent positive charge and discharge curve after “activation”,(c,d) MoS3 equivalent positive electrode electrochemical performance curves[34]
图3 NiS2/FeS用作LSBs等效正极的电化学性能[36]
Fig. 3 Electrochemical performance of NiS2/FeS as equivalent positive electrode of LSBs[36]
图4 NiS2/S共正极材料的表征[39]
Fig. 4 Characterization and performance of NiS2/S cathode[39]
表1 不同过渡金属硫/氧化物电导率对比表
Table 1 Different transition-metal sulfide/oxide conductivity
TMSs Conductivity(S/cm) ref
FeS 80 36
Ni3S2 1.8×10-5 49
Co9S8 2.9×102 46
CuS 8.7×102 49
CoS2 6.7×103 33
Graphene 106 50
Graphene oxide 1.7×102 50
MoS2 3.1 47
Fe3O4 4.0×10-3 51
NiO 10-13 55
V2O5 3.7×10-2 45
TiO2 10-10 17
CoO 2.0×10-4 33
Ti4O7 3.2 48
MnO2 10-5 48
WS2 6.7 52
TiS2 30~50 53
VS2 0.1 17
FeS2 0.6 54
Graphite 1~1000 33
表2 过渡金属硫化物对LiPSs结合能表
Table 2 Binding energy of transition-metal sulfides to LiPSs
TMSs Crystal face LiPSs Binding energy(eV) ref
Co9S8 (002) Li2S2 2.22 35
(202) 3.29
(008) 6.06
Co3S4 (111) Li2S4 2.26 33
Li2S6 1.61
Li2S8 1.68
(220) Li2S4 2.76
Li2S6 2.18
Li2S8 2.18
CoS2 (111) Li2S4 1.97 64
Li2S6 1.01
TiS2 Li2S 2.99
Li2S6 1.02
MoS2 Li2S2 0.82 43
NbS2 Li2S2 0.76
FeS Li2S6 0.87 60, 57
SnS2 Li2S6 0.80 62
VS2 Li2S6 1.04 62
NiS2 (111) Li2S4 2.06 35
Ni3S2 Li2S6 0.72 60
WS2 S8 0.30 27
Li2S8 0.52
Li2S6 0.85
Li2S4 0.80
Li2S2 1.05
Li2S 1.45
ZrS2 Li2S2 2.70 59
TiO2 Li2S 1.66
Graphene Li2S4 0.34 35
Graphite Li2S 0.60
图5 元素对结合能的影响[61]
Fig. 5 Effect of elements on binding energy[61]
图6 过渡金属硫化物对LiPSs的吸附实验图[33,62,63]
Fig. 6 Adsorption test of transition metal sulfides on LiPSs[33,62,63]
图7 金属硫化物对LiPSs的吸附能:(a)Ni3S2对不同LiPSs吸附能的吸附能,(b)不同金属硫化物对不同类型LiPSs吸附能,(c)不同晶面结构硫化物对LiPSs吸附能[35,63]
Fig. 7 Adsorption energy of transition metal sulfides to LiPSs:(a)Adsorption energy of Ni3S2 for adsorption energy of different LiPSs,(b)Adsorption energy of different metal sulfides for different types of LiPSs,(c)Adsorption energy of LiPSs by sulfides of different crystal plane structures[35,63]
图8 TMSs对LiPSs的吸附模型示意图:(a)物理模型[66],(b)化学模型[67]
Fig. 8 Schematic diagram of the adsorption model of TMSs on LiPSs:(a) physical model[66],(b) chemical model[67]
图9 极性导体材料在增强电化学反应动力学中的作用[68,69]
Fig. 9 The role of polar conductor materials in enhancing electrochemical reaction kinetics[68,69]
图10 CoS2添加对氧化还原反应催化作用示意图[33]
Fig. 10 Schematic diagram of the catalytic action of CoS2 on redox reaction[33]
图11 各种金属硫化物表面的锂离子扩散特性及机理分析:(a)氧化过程CV峰值电流与扫描速率的平方根,(b)各种金属硫化物扩散过程的能量分布,(c)不同复合电极在0.5 C下300次循环的循环性能和库仑效率[62]
Fig. 11 Lithium ion diffusion properties on the surface of various metal sulfides with mechanism analysis:(a)oxidation process versus the square root of the scan rates,(b)energy profiles for diffusion processes of Li ion on Ni3S2, SnS2, FeS, CoS2, VS2, TiS2, and graphene and(c)cycling performance and coulombic efficiency of the different composite electrodes at 0.5 C for 300 cycles[62]
表3 TMSs作为LSBs不同组件的数据报告
Table 3 Data report of TMSs as different components in LSBs
TMSs Initial capacity
(mAh·g-1)		 Sulfur loading
(mg·cm-2)		 ref
CoS2 interlayer 1240 at 0.2 C 1.55 70
CoS2 additive 1326 at 0.1 C 2.3 33
Co9S8 host 1130 at 0.05 C 1.5 37
Co9S8-Celgard 1385 at 0.1 C 2.0 71
TiS2 additive 1000 at 0.1 C N/A 22
TiS2 encapsulation 1156 at 0.2 C 2 17
MoS2 additive 1270 at 0.2 C 2 72
MoS2 coating 950 at 0.2 C N/A 73
NiS2 additive 1203 at 0.1 C 2.0~3.3 25
WS2 host 1581 at 0.1 C 2 28
WS2 interlayer 1454 at 0.02 C 4 74
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