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化学进展 2021, Vol. 33 Issue (9): 1665-1678 DOI: 10.7536/PC201215 前一篇   

• 综述 •

碳基材料修饰聚烯烃隔膜提高锂硫电池性能研究

刘新叶1, 梁智超1, 王山星1, 邓远富1,*(), 陈国华2   

  1. 1 华南理工大学化学化工学院 广东省燃料电池技术重点实验室 广州 510641
    2 香港理工大学机械工程系 香港九龙
  • 收稿日期:2020-12-09 修回日期:2021-01-19 出版日期:2021-09-20 发布日期:2021-03-04
  • 通讯作者: 邓远富
  • 基金资助:
    国家自然科学基金-香港RGC项目(21661162002); 国家自然科学基金-香港RGC项目(N_HKUST601/16); 广东省重点研究计划项目(2019B090908001)
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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:2020-12-09 Revised:2021-01-19 Online:2021-09-20 Published:2021-03-04
  • 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)

采用硫单质作正极和金属锂为负极组成的锂硫(Li-S)电池具有很高的理论比能量(2600 Wh·kg-1),被认为是一种具有广泛应用前景的二次电池。其中,正极硫具有高的理论比容量(1675 mAh·g-1),储量丰富且环境友好。然而,硫较差的导电性、多硫化物的穿梭效应和锂枝晶生长等导致了Li-S电池在循环过程中容量衰减快、库仑效率低和安全隐患等问题,严重阻碍了其大规模应用。通过隔膜修饰提高Li-S电池的性能是一种有效的方法,近年来取得了很大进展。碳材料是较常见的一种隔膜修饰材料,本文综述了近年来常见碳材料及碳基复合材料用于修饰Li-S电池隔膜进而改善电池性能方面的研究进展,重点介绍了修饰层的设计及提升Li-S电池容量的机理。

关键词： Li-S电池, 隔膜修饰, 电化学性能改善, 穿梭效应, 催化

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
()
图1 (a)Li-S电池充放电曲线[5];(b)穿梭效应示意图[6]
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
表1 利用碳材料修饰的隔膜组装的Li-S电池的性能对比
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
图2 (a)采用多孔碳纸作为中间层阻止多硫化物扩散的示意图[20];(b)采用石墨烯修饰的PP隔膜组装成的Li-S电池的示意图[26];(c)多孔氧化镁模板上采用CVD法制备PG的示意图和PG隔膜抑制穿梭效应原理的示意图[27];(d)用不同氧化程度的GO改性的复合膜的Li-S电池的循环性能图[34];(e)G@PC/PP隔膜合成的示意图[44];(f)由蟹壳合成N掺杂多孔碳步骤图以及修饰隔膜捕获多硫化锂的原理示意图[53]
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
图3 (a)使用MTO-CNTs中间层的锂电池结构示意图[63];(b)使用rGO@MoS2修饰隔膜用于Li-S电池示意图和rGO@MoS2的扫描电镜图[71];(c)多硫化物在TiN, TiO2和TiO2-TiN异质结构表面的转换过程示意图[73];(d)Mo2C@NG的制备和作用机理示意图[78]
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
图4 (a)合成N-Ti3C2/C纳米片改性PP隔膜示意图[81];(b)合成Ni@NG及其结构示意图[90];(c)采用双层rGO-PVDF/PVDF修饰隔膜的示意图[98];(d)采用g-C3N4/GS中间层用于正极表面的Li-S电池示意图[99]
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
表2 利用复合材料修饰隔膜组装的Li-S电池的性能对比
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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