Steric Hindrance-Induced Amorphous Lithium Sulfide Deposition Accelerates Sulfur Redox Kinetics in Lithium-Sulfur Batteries
Wang, Zhihua; Ke, Junru; Zhu, He; Xue, Fan; Jiang, Jun; Huang, Wen; Dong, Min; Zhu, Xindong; Zeng, Jianrong; Song, Ruoyu; Sliz, Rafal; Ji, Qingmin; Liu, Qi; Fu, Yongsheng; Lan, Si (2025-05-13)
Avaa tiedosto
Sisältö avataan julkiseksi: 13.05.2026
Wiley-VCH Verlag
13.05.2025
Z. Wang, J. Ke, H. Zhu, F. Xue, J. Jiang, W. Huang, M. Dong, X. Zhu, J. Zeng, R. Song, R. Sliz, Q. Ji, Q. Liu, Y. Fu, S. Lan, Steric Hindrance-Induced Amorphous Lithium Sulfide Deposition Accelerates Sulfur Redox Kinetics in Lithium–Sulfur Batteries. Adv. Mater. 2025, 2504715. https://doi.org/10.1002/adma.202504715
https://rightsstatements.org/vocab/InC/1.0/
© 2025 Wiley-VCH GmbH. This is the peer reviewed version of the following article: Z. Wang, J. Ke, H. Zhu, F. Xue, J. Jiang, W. Huang, M. Dong, X. Zhu, J. Zeng, R. Song, R. Sliz, Q. Ji, Q. Liu, Y. Fu, S. Lan, Steric Hindrance-Induced Amorphous Lithium Sulfide Deposition Accelerates Sulfur Redox Kinetics in Lithium–Sulfur Batteries. Adv. Mater. 2025, 2504715, which has been published in final form at https://doi.org/10.1002/adma.202504715. This article may be used for non-commercial purposes in accordance with Wiley Terms and Conditions for Use of Self-Archived Versions. This article may not be enhanced, enriched or otherwise transformed into a derivative work, without express permission from Wiley or by statutory rights under applicable legislation. Copyright notices must not be removed, obscured or modified. The article must be linked to Wiley’s version of record on Wiley Online Library and any embedding, framing or otherwise making available the article or pages thereof by third parties from platforms, services and websites other than Wiley Online Library must be prohibited.
https://rightsstatements.org/vocab/InC/1.0/
© 2025 Wiley-VCH GmbH. This is the peer reviewed version of the following article: Z. Wang, J. Ke, H. Zhu, F. Xue, J. Jiang, W. Huang, M. Dong, X. Zhu, J. Zeng, R. Song, R. Sliz, Q. Ji, Q. Liu, Y. Fu, S. Lan, Steric Hindrance-Induced Amorphous Lithium Sulfide Deposition Accelerates Sulfur Redox Kinetics in Lithium–Sulfur Batteries. Adv. Mater. 2025, 2504715, which has been published in final form at https://doi.org/10.1002/adma.202504715. This article may be used for non-commercial purposes in accordance with Wiley Terms and Conditions for Use of Self-Archived Versions. This article may not be enhanced, enriched or otherwise transformed into a derivative work, without express permission from Wiley or by statutory rights under applicable legislation. Copyright notices must not be removed, obscured or modified. The article must be linked to Wiley’s version of record on Wiley Online Library and any embedding, framing or otherwise making available the article or pages thereof by third parties from platforms, services and websites other than Wiley Online Library must be prohibited.
https://rightsstatements.org/vocab/InC/1.0/
Julkaisun pysyvä osoite on
https://urn.fi/URN:NBN:fi:oulu-202505193612
https://urn.fi/URN:NBN:fi:oulu-202505193612
Tiivistelmä
Abstract
Lithium–sulfur (Li─S) batteries are promising candidates for next-generation energy storage due to their ultrahigh theoretical energy density. However, their practical application is severely hindered by the sluggish conversion kinetics, particularly during the crystalline lithium sulfide (Li2S) formation stage. Herein, a steric hindrance-mediated engineering strategy is proposed that induces an amorphous Li2S deposition process, effectively boosting the sulfur redox kinetics in Li─S batteries. By introducing benzo-15-crown-5 (B15C5) as an electrolyte additive, a strong coordination between B15C5 and lithium ion (Li+) is established, which creates spatial confinement around Li2S and disrupts the crystallinity of Li2S during its deposition. Synchrotron pair distribution function analysis combined with in situ X-ray diffraction reveals that the deposited Li2S with B15C5 exhibits significant local disorder with irregular Li─S bond oscillations, confirming the generation of an amorphous phase. This strategy not only ensures a uniform Li2S layer at the cathode/electrolyte interface but also lowers the energy barrier of sulfur species at the molecular scale, enabling the Li─S batteries with excellent cycling stability and overall enhanced sulfur reaction kinetics. This work provides a novel pathway for overcoming the intrinsic limitations of sluggish cathode conversion kinetics of Li─S batteries, paving the way for their practical deployment in high-performance energy storage applications.
Lithium–sulfur (Li─S) batteries are promising candidates for next-generation energy storage due to their ultrahigh theoretical energy density. However, their practical application is severely hindered by the sluggish conversion kinetics, particularly during the crystalline lithium sulfide (Li2S) formation stage. Herein, a steric hindrance-mediated engineering strategy is proposed that induces an amorphous Li2S deposition process, effectively boosting the sulfur redox kinetics in Li─S batteries. By introducing benzo-15-crown-5 (B15C5) as an electrolyte additive, a strong coordination between B15C5 and lithium ion (Li+) is established, which creates spatial confinement around Li2S and disrupts the crystallinity of Li2S during its deposition. Synchrotron pair distribution function analysis combined with in situ X-ray diffraction reveals that the deposited Li2S with B15C5 exhibits significant local disorder with irregular Li─S bond oscillations, confirming the generation of an amorphous phase. This strategy not only ensures a uniform Li2S layer at the cathode/electrolyte interface but also lowers the energy barrier of sulfur species at the molecular scale, enabling the Li─S batteries with excellent cycling stability and overall enhanced sulfur reaction kinetics. This work provides a novel pathway for overcoming the intrinsic limitations of sluggish cathode conversion kinetics of Li─S batteries, paving the way for their practical deployment in high-performance energy storage applications.
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