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Progress in Chemistry 2021, Vol. 33 Issue (9): 1665-1678 DOI: 10.7536/PC201215 Previous Articles   

• Review •

Carbon-Based Materials for Modification of Polyolefin Separators to Improve the Performance of Lithium-Sulfur Batteries

Xinye Liu1, Zhichao Liang1, Shanxing Wang1, Yuanfu Deng1(), Guohua Chen2   

  1. 1 The Key Laboratory of Fuel Cell for Guangdong Province, School of Chemistry and Chemical Engineering, South China University of Technology,Guangzhou 510641, China
    2 Department of Mechanical Engineering, The Hong Kong Polytechnic University, Hong Hom Kowloon, China
  • Received: Revised: Online: Published:
  • Contact: Yuanfu Deng
  • Supported by:
    NSFC-RGC Joint Research Scheme(21661162002); NSFC-RGC Joint Research Scheme(N_HKUST601/16); Guangdong Key R&D Program of China(2019B090908001)
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Owing to their great theoretical energy density (2600 Wh·kg-1), lithium-sulfur (Li-S) batteries are one of the most promising candidates of the next generation energy storage devices. Moreover, the high theoretical specific capacity (1675 mAh·g-1), good eco-friendliness, abundant natural resource and low cost of cathode sulfur are also good for the cheap cost and low environmental pollution of Li-S batteries. However, the practical applications of Li-S batteries are severely impeded by several key challenges, such as the low practical specific capacities, low coulomb efficiencies and fast capacity decay, which resulting from the poor electronic conductivity of sulfur and final products Li2S2/Li2S, the shuttle effects of lithium polysulfides and the growth of lithium dendrite during the electrochemical cycling. It is noted that the modification of the polyolefin separators is one of the effective methods to obviously improve the performances of Li-S batteries. In particular, various carbons and their composites are widely used materials for separator modification because of their unique properties, also, many advancements have been achieved. Herein, the research progresses of the various carbons and their composites for separator modification are reviewed, which will provide guidance for the future research on improving the performance of Li-S batteries by separator modification method.

Contents

1 Introduction

2 Carbon materials for separator modification

3 Carbon-based composite materials for separator modification

4 Conclusion and outlook

Key words: lithium-sulfur batteries, separator modification, electrochemical performance improvement, shuttle effect, catalysis
Figure 1 (a) An ideal charge-discharge profile of Li-S batteries[5]. Copyright 2013, Royal Society of Chemistry. (b) Schematic illustration of the parasitic polysulfide shuttle effect in a liquid electrolyte based Li-S batteries[6]. Copyright 2014, Elsevier
Table 1 Detailed information of Li-S batteries with modified separators by carbon-based materials
Separator
coating materials		 Separator coating loading
(mg·cm-2)		 Separator coating thickness (μm) Cathode S content (%) Cathode S loading
(mg·cm-2)		 1st Cycling data (mAh·g-1) nth Cycling data (mAh·g-1) and C-rate Fading (%) at nth cycles ref
Active carbon paper 70 1367@0.5 C >1000 (1 C, 100 cycles) 0.15 20
Super P 0.2 ~20 60 1.1~1.3 1289@0.5 C 810 (0.5 C, 200 cycles) 0.19 22
KB+Super P 0.18 10 80 1318@0.1 C 815 (1 C, 100 cycles) 24
G@PP 1.3 30 70 1.5~2.1 1278@0.3 A·g-1 633 (1.5 A·g-1, 500 cycles) 0.064 26
G(CVD) 0.54 ~10 63 1.8~2 1449@0.05 C 877 (0.5 C, 150 cycles) 27
GO 0.75 70 1~1.2 1063@0.5 C 834 (0.5 C, 100 cycles) 0.21 33
Partially reduced GO ~1 80 ~900@0.1 C 450 (0.2 C, 50 cycles) 34
N-doped MPC 0.5 24 70 3.95 1364@0.2 C 566 (0.5 C, 1200 cycles) 0.04 36
G@PC 0.075 0.9 64 3.5 851@1 C 754 (1 C, 500 cycles) 0.023 44
NEPC 0.364 16 1.5 1328@0.2 C 464 (0.5 C, 550 cycles) 0.088 52
N-MLMEC 0.2 4 63 1.5~2.0 1301@0.1 C 971.3(0.1 C, 100 cycles) 0.25 53
CBC 81 1.2~1.6 1134@0.2 A·g-1 620 (0.8 A·g-1, 300 cycles) 46
Fig. 2 (a) Schematic configuration of a Li-S cell with a bifunctional microporous carbon interlayer inserted between the sulfur cathode and the separator[20]; Copyright 2012, Nature. (b) Schematic of the electrode configuration using an integrated structure of sulfur and G@PP separator and the corresponding battery assembly[26]; Copyright 2015, Wiley. (c) Schematic illustration of PG fabrication though methane CVD on porous MgO templates and schematic illustration of difference between PP and PG separators in effecting cathode/separator interfaces[27]; Copyright 2017, Elsevier. (d) Cycling stability of cell with different GO modified separator[34]; (e) Schematic illustration of the synthesis of the G@PC/PP separator in Li-S batteries[44]; Copyright 2018, Elsevier. (f) Synthesis of the N-MIMEC from crab shells and the LiPS-trapping mechanisms of the N-MIMEC-coated separator during discharge/charge process[53]. Copyright 2017, Royal Society of Chemistry
Fig. 3 (a) Schematic cell configuration of Li-S batteries using MTO-CNTs interlayer[63]; Copyright 2019, Elsevier. (b) The schematic Li-S cell with rGO@MoS2 coated separator, and SEM image of rGO@MoS2 composite[71]; Copyright 2017, Royal Society of Chemistry. (c) Schematic of LiPS conversion processes on TiN, TiO2 and the TiO2-TiN heterostructure surface[73]; Copyright 2016, Royal Society of Chemistry. (d) Schematic illustration of the preparation of Mo2C@NG nanocomposite[78]. Copyright 2020, Elsevier
Fig. 4 (a) Schematic illustration for the synthesis of N-Ti3C2/C nanosheets and the modified PP separator for Li-S batteries[81]; Copyright 2019, Elsevier. (b) Schematic illustration of the preparation of Ni@NG with the Ni-N4 sites[90]; Copyright 2016, Wiley. (c) Schematic illustration of bifunctional double layer rGO-PVDF/PVDF membrane separator[98]; Copyright 2017, Royal Society of Chemistry. (d) Schematic of cell configuration with a laminated structure g-C3N4/GS cathode interlayer[99]. Copyright 2019, Wiley
Table 2 Detailed information of Li-S batteries with modified separators by composite materials
Separator
coating materials		 Separator coating loading (mg·cm-2) Separator coating thickness (μm) Cathode S content (%) Cathode S
loading
(mg·cm-2)		 1st Cycling data
(mAh·g-1)		 nth Cycling data (mAh·g-1) and C-rate Fading (%) at nth cycles ref
Al2O3/CNT 17 42 1 1287@0.2 C 807 (0.2 C, 200 cycles) 0.37 58
MoS2/CNT 0.25 2 50 1.4 1237@0.5 C 648 (0.5 C, 500 cycles) 0.061 60
TiO2/SiO2/CNF 0.4 10 72.7 ~1.8 1329@0.1 C 435 (2 C, 500 cycles) 0.06 65
mTiO2-CNTs 0.06 8 65 1.1 1212@0.2 C 577 (0.5 C, 500 cycles) 0.07 63
CNFO@CNT 1.25 60 1 1332@0.1 C 755(2 C, 250 cycles) 0.063 64
SnO2/rGO 0.15 20 55 2.87 1076@0.5 C 602 (2 C, 200 cycles) 68
MnO2/rGO ~0.8 1 70 1.8~2.0 1460@0.1 C 480 (1 C, 300 cycles) 0.07 67
rGO@MoS2 0.24 8 70 1.8~2.0 1122@0.2 C 603 (1 C, 500 cycles) 0.116 71
TiO2-TiN/G 0.23 9 1.0~1.2 >1200@0.1 C 927 (0.3 C, 300 cycles) 0.027 73
TiC/G 0.46 21 85 1.1~1.4 1255@0.1 C 765 (0.3 C, 200 cycles) 75
MQD@NG 11.5 80 2.1 1230@0.2 C 823 (1 C, 200 cycles) 0.045 78
Nb2O5-rGO
Mo2C@NG		 0.05 0.2 75 1 1328@0.2 C 378.4 (3 C, 500 cycles) 79
N-Ti3C2/C 0.6 6 64 3.4 1111@0.2 C 716 (0.5 C, 500 cycles) 0.07 81
Co/NCNS/CNT ~0.2 5.94 64 2 1253@0.1 C 434 (2 C, 1000 cycles) 0.05 82
Ni@NG 0.3 13.5 1.5 1598@0.1 C 826.2 (1 C, 500 cycles) 0.044 90
Fe1/NG 0.1 7 4.5 ~1200@0.2 C 892 (0.5 C, 750 cycles) 92
GO/Nafion 0.053 0.13 60 1.2 1090@0.1 C 651 (0.5 C, 200 cycles) 0.18 94
rGO-PVDF 95 70 1.1 1322@0.2 C 646 (0.2 C, 200 cycles) 0.25 98
g-C3N4/GS ~15 45 0.9~1.1 1350@0.1 C 612.4 (1 C, 1000 cycles) 99
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