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A novel insight into deterioration of heavily sulfur-loaded cathode in Li-S battery

Ye, Ke Fen and Xia, Yin Ping and Liu, Rui and Liu, Bin Hong and Li, Zhou Peng (2022) A novel insight into deterioration of heavily sulfur-loaded cathode in Li-S battery. Electrochimica Acta, 435 . Art. No. 141387. ISSN 0013-4686. doi:10.1016/j.electacta.2022.141387.

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Active-substance (S₈ and Li₂S) deposition layer formed on polar interfaces is more reactive than that formed on apolar interfaces. However, when deposition layer reaches a certain thickness, by-path active-substance deposition takes place because of polysulfide disproportionation, which aggravates active-substance segregation to decrease the reactivity. This leads to a significant capacity decay and failure to accomplish polysulfide delithiation after certain cycles, which is understood as the results of decreased active-substance utilization and formed local micro-short-circuits, respectively. The finding of correlation between active-substance segregation and cathode deterioration inspires the design of polytetrafluoroethylene-based self-supported cathode to suppress active-substance segregation through avoiding increase of interphase contact resistance during cycling. With S-loading of 4.0 mg cm⁻², the as-prepared cathode demonstrates excellent cycleability, retaining a capacity of 300 mAh g⁻¹ at a rate of 2C after 1000 cycles. When increasing S-loading up to 36.5 mg cm⁻², the as-obtained cathode delivers an ultra-high areal capacity of 24.6 mAh cm⁻² after 100 cycles at 0.1 C. However, increasing S-loading aggravates Li₂S segregation which then narrows down Li⁺ transportation, leading to formation and growth of Li-shunts which in turn stimulates active-substance segregation. Such an inductive interaction between Li-shunt growth and active-substance segregation results in the fast formation of local micro-short-circuits, causing the constant supply of Li from Li shunts to cathode, and eventually accelerating cathode deterioration.

Item Type:Article
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URLURL TypeDescription
Ye, Ke Fen0000-0001-6476-6919
Li, Zhou Peng0000-0003-3176-628X
Additional Information:This work is financially supported by the National Natural Science Foundation of China, Grant Nos. 21978261 and 21776245.
Funding AgencyGrant Number
National Natural Science Foundation of China21776245
National Natural Science Foundation of China21978261
Record Number:CaltechAUTHORS:20221128-494241100.42
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Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:118080
Deposited By: Research Services Depository
Deposited On:20 Dec 2022 18:03
Last Modified:20 Dec 2022 18:03

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