复合导电添加剂对全固态锂硫电池性能影响的研究

doi:10.13208/j.electrochem.200527

电化学（中英文） ›› 2021, Vol. 27 ›› Issue (4): 388-395. doi: 10.13208/j.electrochem.200527

复合导电添加剂对全固态锂硫电池性能影响的研究

王东浩, 晏鹤凤, 龚正良^*()

厦门大学能源学院,福建厦门 361005

收稿日期:2020-05-27 修回日期:2020-07-16 出版日期:2021-08-28 发布日期:2020-07-17
通讯作者: 龚正良 E-mail:zlgong@xmu.edu.cn
基金资助:
国家自然科学基金项目(21875196);国家自然科学基金项目(21935009);福建省引导性计划项目(2019H0003);厦门大学大学生创新创业训练计划项目(201810384171)

Effect of Conductive Additives on Electrochemical Performance of All-Solid-State Li-S Batteries

Dong-Hao Wang, He-Feng Yan, Zheng-Liang Gong^*()

College of Energy, Xiamen University, Xiamen 361005, Fujian, China

Received:2020-05-27 Revised:2020-07-16 Published:2021-08-28 Online:2020-07-17
Contact: Zheng-Liang Gong E-mail:zlgong@xmu.edu.cn

摘要/Abstract

摘要：

使用硫化物固体电解质的全固态锂硫电池由于多硫化物不溶于硫化物固体电解质及硫化物电解质不可燃的特性,得以完全避免穿梭效应并显著提高了电池的安全性能而被认为是极具潜力的下一代储能电池。如何建立并平衡复合正极中离子/电子导电网络且维持复合正极中较高活性物质含量对于全固态锂硫电池至关重要。本文以单质硫为活性物质研究了复合导电添加剂对全固态锂硫电池性能的影响,发现以乙炔黑（AB）为导电碳材料明显优于Super P和Ketjen Black;优化复合正极的组成,发现硫：乙炔黑：固体电解质的质量比为40:20:40时,全固态锂硫电池在室温和60℃下均具有良好的电化学性能。

关键词: 全固态锂硫电池, 复合硫正极, 电子/离子输运, 高硫含量

Abstract:

All-solid-state lithium sulfur batteries (ASSLSBs) with inorganic solid electrolytes offer an opportunity to realize both high energy density (lithium metal ~ 3860 mAh·g^-1, sulfur ~ 1675 mAh·g^-1), safety and reliability, via eliminating the polysulfides shuttle effect and flammable liquid electrolyte. However, it still remains a huge challenge for ASSLSBs to achieve high areal active mass loading, high utilization efficiency of the active materials and good cycle stability simultaneously due to the insulating nature of sulfur and Li₂S (conductivities of sulfur and Li₂S are 5×10^-30 S·cm^-1 and 3.6×10^-7 S·cm^-1 at room temperature, respectively), and the large volume change during cycling due to the difference in mass density between sulfur (2.03 g·cm^-3) and Li₂S (1.67 g·cm^-3). Herein, Li₇P₃S₁₁ (LPS) glass-ceramic sulfide solid electrolyte with high ionic conductivity of 1.7×10^-3 S·cm^-1 at room temperature was synthesized through high energy ball-milling and a two-step heat treatment. And the effect of conductive additives on electrochemical performance of ASSLSBs employing sulfur as an active material and LPS as a solid electrolyte was systematically investigated. It shows that ASSLSBs employing acetylene black (AB) as a conductive additive exhibited much better electrochemical performance with high capacity of 1681 mAh·g^-1 and good rate performance at 60℃ than Super P and Ketjen Black. ASSLBs employing sulfur composite cathode with the optimized mass ratio of S:AB:solid electrolyte = 4:2:4 presented the best electrochemical performance at both room temperature and 60℃. ASSLBs employing S₄₀-AB₂₀-LPS₄₀ composite cathode delivered a high capacity of 1450 mAh·g^-1 with good cycling stability and high coulombic efficiency of ~100% at 60℃. And good electrochemical performance could also be obtained even at room temperature. A high initial discharge capacity of ~1270 mAh·g^-1 was obtained and a high capacity of 1140 mAh·g^-1 was retained after 30 cycles with high coulombic efficiency of ~100%.

Key words: all-solid-state lithium sulfur battery, composite sulfur cathode, electron/ion transport, high sulfur content

王东浩, 晏鹤凤, 龚正良. 复合导电添加剂对全固态锂硫电池性能影响的研究[J]. 电化学（中英文）, 2021, 27(4): 388-395.

Dong-Hao Wang, He-Feng Yan, Zheng-Liang Gong. Effect of Conductive Additives on Electrochemical Performance of All-Solid-State Li-S Batteries[J]. Journal of Electrochemistry, 2021, 27(4): 388-395.

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Content of active material	Content of S/%	Content of AB/%	Content of LPS/%	Capacity/ (mAh·g(sulfur)^-1)	Capacity/ (mAh·g(cathode)^-1)
25%	25	25	50	1850	462
30%	30	30	40	950	285
35%	35	25	40	1300	455
40%	40	20	40	1450	580
45%	45	20	35	1050	472
50%	50	20	30	1050	525

复合导电添加剂对全固态锂硫电池性能影响的研究

Effect of Conductive Additives on Electrochemical Performance of All-Solid-State Li-S Batteries

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