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Nano Research 2023, 16(10): 12035-12042 https://doi.org/10.1007/s12274-022-5061-4
Research Article | Issue | Published: 12 November 2022

Theoretical kinetic quantitative calculation predicted the expedited polysulfides degradation

Show Author's Information Siyu Zhang1,  Xianchao Rong1,  Tao Li2,  Wenjie Ren1,  Hao Ren1( ),  Linjie Zhi1,  Mingbo Wu1( ),  Zhongtao Li1( )
State Key Laboratory of Heavy Oil Processing, College of Chemical Engineering, China University of Petroleum (East China), Qingdao 266580, China
National Engineering Center of Coal slurry and Coal Chemical Co., Ltd., LTD, Jinan 250014, China
Keywords:
lithium-sulfur batteries, first-principles calculation, shuttle effect, polysulfide degradation, semi-empirical model
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Zhang S, Rong X, Li T, et al. Theoretical kinetic quantitative calculation predicted the expedited polysulfides degradation. Nano Research, 2023, 16(10): 12035-12042. https://doi.org/10.1007/s12274-022-5061-4
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Abstract Full text Electronic supplementary material About this article

The performance of lithium-sulfur battery is restricted by the lower value of electrode conductance and the sluggish LiPSs degradation kinetics. Unfortunately, the degradation rate of polysulfides was mostly attributed to the catalytic energy barrier in previous, which is unable to give accurate predictions on the performance of lithium-sulfur battery. Thereby, a quantitative framework relating the battery performance to catalytic energy barrier and electrical conductivity of the cathode host is developed here to quantitate the tendency. As the model compound, calculated-Ti4O7 (c-Ti4O7) has the highest comprehensive index with excellent electrical conductivity, although the catalytic energy barrier is not ideal. Through inputting the experimental properties such as impedance and charge/discharge data into the as-build model, the final conclusion is still in line with our prediction that Ti4O7 host shows the most excellent electrochemical performance. Therefore, the accurate model here would be attainable to design lithium-sulfur cathode materials with a bottom–up manner.


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Electronic supplementary material
About this article

Theoretical kinetic quantitative calculation predicted the expedited polysulfides degradation

Show Author's information Siyu Zhang1, Xianchao Rong1, Tao Li2, Wenjie Ren1, Hao Ren1( ), Linjie Zhi1, Mingbo Wu1( ), Zhongtao Li1( )
State Key Laboratory of Heavy Oil Processing, College of Chemical Engineering, China University of Petroleum (East China), Qingdao 266580, China
National Engineering Center of Coal slurry and Coal Chemical Co., Ltd., LTD, Jinan 250014, China

Abstract

The performance of lithium-sulfur battery is restricted by the lower value of electrode conductance and the sluggish LiPSs degradation kinetics. Unfortunately, the degradation rate of polysulfides was mostly attributed to the catalytic energy barrier in previous, which is unable to give accurate predictions on the performance of lithium-sulfur battery. Thereby, a quantitative framework relating the battery performance to catalytic energy barrier and electrical conductivity of the cathode host is developed here to quantitate the tendency. As the model compound, calculated-Ti4O7 (c-Ti4O7) has the highest comprehensive index with excellent electrical conductivity, although the catalytic energy barrier is not ideal. Through inputting the experimental properties such as impedance and charge/discharge data into the as-build model, the final conclusion is still in line with our prediction that Ti4O7 host shows the most excellent electrochemical performance. Therefore, the accurate model here would be attainable to design lithium-sulfur cathode materials with a bottom–up manner.

Keywords: lithium-sulfur batteries, first-principles calculation, shuttle effect, polysulfide degradation, semi-empirical model

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Publication history
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Acknowledgements

Publication history

Received: 08 August 2022
Revised: 11 September 2022
Accepted: 14 September 2022
Published: 12 November 2022
Issue date: October 2023

Copyright

© Tsinghua University Press 2022

Acknowledgements

This work was supported by the Natural Science Foundation of Shandong, China (Nos. ZR2020JQ21 and ZR2021ZD24), the National Natural Science Foundation of China (Nos. 51873231 and 22138013), the Financial Support from Taishan Scholar Project (No. tsqn201909062), the Technology Foundation of Shandong Energy Group Co., LTD. (Nos. YKZB2020-176 and J2020004), and the Fundamental Research Funds for the Central Universities (No. 20CX05010A).

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