Accelerating Sulfur Redox Kinetics by Electronic Modulation and Drifting Effects of Pre‐Lithiation Electrocatalysts

Accelerating Sulfur Redox Kinetics by Electronic Modulation and Drifting Effects of Pre‐Lithiation Electrocatalysts

Advanced Materials

10.1002/adma.202307741

http://dx.doi.org/10.1002/adma.202307741

Haimei Wang, Hao Yuan, Wanwan Wang, Xingyang Wang, Jianguo Sun, Jing Yang, Ximeng Liu, Qi Zhao, Tuo Wang, Ning Wen, Yulin Gao, Kepeng Song, Dairong Chen, Shijie Wang, Yong‐Wei Zhang, John Wang

10 October 2023

Wang, H., Yuan, H., Wang, W., Wang, X., Sun, J., Yang, J., Liu, X., Zhao, Q., Wang, T., Wen, N., Gao, Y., Song, K., Chen, D., Wang, S., Zhang, Y., & Wang, J. (2023). Accelerating Sulfur Redox Kinetics by Electronic Modulation and Drifting Effects of Pre‐Lithiation Electrocatalysts. Advanced Materials, 36(8). Portico. https://doi.org/10.1002/adma.202307741

AbstractEfficient catalyst design is crucial for addressing the sluggish multi‐step sulfur redox reaction (SRR) in lithium‐sulfur batteries (LiSBs), which are among the promising candidates for the next‐generation high‐energy‐density storage systems. However, the limited understanding of the underlying catalytic kinetic mechanisms and the lack of precise control over catalyst structures pose challenges in designing highly efficient catalysts, which hinder the LiSBs’ practical application. Here, drawing inspiration from the theoretical calculations, the concept of precisely controlled pre‐lithiation SRR electrocatalysts is proposed. The dual roles of channel and surface lithium in pre‐lithiated 1T’‐MoS2 are revealed, referred to as the “electronic modulation effect” and “drifting effect”, respectively, both of which contribute to accelerating the SRR kinetics. As a result, the thus‐designed 1T’‐LixMoS2/CS cathode obtained by epitaxial growth of pre‐lithiated 1T’‐MoS2 on cubic Co9S8 exhibits impressive performance with a high initial specific capacity of 1049.8 mAh g−1, excellent rate‐capability, and remarkable long‐term cycling stability with a decay rate of only 0.019% per cycle over 1000 cycles at 3 C. This work highlights the importance of precise control in pre‐lithiation parameters and the synergistic effects of channel and surface lithium, providing new valuable insights into the design and optimization of SRR electrocatalysts for high‐performance LiSBs.

Publisher Copyright

This research / project is supported by the National Research Foundation - Competitive Research Programme
Grant Reference no. : NRF-CRP26-2021-0003

This research / project is supported by the A*STAR - SERC Central Research Fund (CRF)
Grant Reference no. : NA

support from the Italy-Singapore Science and Technology Cooperation (Grant No. R23101R040)

This is the peer reviewed version of the following article: Wang, H., Yuan, H., Wang, W., Wang, X., Sun, J., Yang, J., Liu, X., Zhao, Q., Wang, T., Wen, N., Gao, Y., Song, K., Chen, D., Wang, S., Zhang, Y., & Wang, J. (2023). Accelerating Sulfur Redox Kinetics by Electronic Modulation and Drifting Effects of Pre‐Lithiation Electrocatalysts. Advanced Materials, 36(8). Portico. https://doi.org/10.1002/adma.202307741 , which has been published in final form at doi.org/10.1002/adma.202307741. 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://oar.a-star.edu.sg/communities-collections/articles/19890

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