Citation: Qihou Li, Jiamin Liu, Fulu Chu, Jinwei Zhou, Jieshuangyang Chen, Zengqiang Guan, Xiyun Yang, Jie Lei, Feixiang Wu. Coordinating lithium polysulfides to inhibit intrinsic clustering behavior and facilitate sulfur redox conversion in lithium-sulfur batteries[J]. Chinese Chemical Letters, ;2025, 36(5): 110306. doi: 10.1016/j.cclet.2024.110306 shu

Coordinating lithium polysulfides to inhibit intrinsic clustering behavior and facilitate sulfur redox conversion in lithium-sulfur batteries

Qihou Li ^a ,
Jiamin Liu ^{a, *,} ,
Fulu Chu ^{a, c} ,
Jinwei Zhou ^a ,
Jieshuangyang Chen ^a ,
Zengqiang Guan ^a ,
Xiyun Yang ^a ,
Jie Lei ^{b, *,} ,
Feixiang Wu ^{a, *,}

a.
School of Metallurgy and Environment, National Engineering Research Centre of Advanced Energy Storage Materials, Central South University, Changsha 410083, China
b.
College of Materials Science and Engineering, Institute of New Energy Materials and Engineering, Fuzhou University, Fuzhou 350108, China
c.
School of Materials Science & Engineering, University of Jinan, Ji'nan 250022, China

liujiamin_2023@163.com

jielei@fzu.edu.cn

feixiang.wu@csu.edu.cn

Received Date: 2 June 2024
Revised Date: 2 July 2024
Accepted Date: 30 July 2024
Available Online: 31 July 2024

Figures(5)

The intrinsic clustering behavior and kinetically sluggish conversion process of lithium polysulfides seriously limit the electrochemical reversibility of sulfur redox reactions in lithium-sulfur (Li-S) batteries. Here, we introduce molybdenum pentachloride (MoCl₅) into the electrolyte which could coordinate with lithium polysulfides and inhibit their intrinsic clustering behavior, subsequently serving as an improved mediator with the bi-functional catalytic effect for Li₂S deposition and activation. Moreover, the coordination bonding and accelerated conversion reaction can also greatly suppress the dissolution and shuttling of polysulfides. Consequently, such polysulfide complexes enable the Li-S coin cell to exhibit good long-term cycling stability with a capacity decay of 0.078% per cycle after 400 cycles at 2 C, and excellent rate performance with a discharge capacity of 589 mAh/g at 4 C. An area capacity of 3.94 mAh/cm² is also achieved with a high sulfur loading of 4.5 mg/cm² at 0.2 C. Even at -20 ℃, the modified cell maintains standard discharge plateaus with low overpotential, delivering a high capacity of 741 mAh/g at 0.2 C after 80 cycles. The low-cost and convenient MoCl₅ additive opens a new avenue for the effective regulation of polysulfides and significant enhancement in sulfur redox conversion.
- Lithium-sulfur (Li-S) battery,
- Polysulfide clustering,
- Coordinating reaction,
- Improved mediator,
- Shuttle effect
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