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Progress in Chemistry 2019, Vol. 31 Issue (8): 1166-1176 DOI: 10.7536/PC190140 Previous Articles   Next Articles

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: Online: Published:
  • 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)
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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
Fig. 1 Schematic diagram of the effect of transition metal sulfides on the promotion of LSBs
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]
Fig. 3 Electrochemical performance of NiS2/FeS as equivalent positive electrode of LSBs[36]
Fig. 4 Characterization and performance of NiS2/S cathode[39]
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
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
Fig. 5 Effect of elements on binding energy[61]
Fig. 6 Adsorption test of transition metal sulfides on LiPSs[33,62,63]
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]
Fig. 8 Schematic diagram of the adsorption model of TMSs on LiPSs:(a) physical model[66],(b) chemical model[67]
Fig. 9 The role of polar conductor materials in enhancing electrochemical reaction kinetics[68,69]
Fig. 10 Schematic diagram of the catalytic action of CoS2 on redox reaction[33]
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]
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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