Version 1
: Received: 19 April 2024 / Approved: 19 April 2024 / Online: 19 April 2024 (15:23:37 CEST)
How to cite:
Feng, S.; Yin, T.; Bian, L.; Liu, Y.; Cheng, T. Optimization of Lithium Metal Anode Performance: Investigating the Interfacial Dynamics and Reductive Mechanism of Asymmetric Sulfonylimide Salts. Preprints2024, 2024041356. https://doi.org/10.20944/preprints202404.1356.v1
Feng, S.; Yin, T.; Bian, L.; Liu, Y.; Cheng, T. Optimization of Lithium Metal Anode Performance: Investigating the Interfacial Dynamics and Reductive Mechanism of Asymmetric Sulfonylimide Salts. Preprints 2024, 2024041356. https://doi.org/10.20944/preprints202404.1356.v1
Feng, S.; Yin, T.; Bian, L.; Liu, Y.; Cheng, T. Optimization of Lithium Metal Anode Performance: Investigating the Interfacial Dynamics and Reductive Mechanism of Asymmetric Sulfonylimide Salts. Preprints2024, 2024041356. https://doi.org/10.20944/preprints202404.1356.v1
APA Style
Feng, S., Yin, T., Bian, L., Liu, Y., & Cheng, T. (2024). Optimization of Lithium Metal Anode Performance: Investigating the Interfacial Dynamics and Reductive Mechanism of Asymmetric Sulfonylimide Salts. Preprints. https://doi.org/10.20944/preprints202404.1356.v1
Chicago/Turabian Style
Feng, S., Yue Liu and Tao Cheng. 2024 "Optimization of Lithium Metal Anode Performance: Investigating the Interfacial Dynamics and Reductive Mechanism of Asymmetric Sulfonylimide Salts" Preprints. https://doi.org/10.20944/preprints202404.1356.v1
Abstract
Asymmetric lithium salts, such as Lithium (difluoromethanesulfonyl)(trifluoromethanesulfonyl)imide (LiDFTFSI), have been demonstrated to surpass traditional symmetric lithium salts with improved Li+ conductivity and the capacity to generate stable solid electrolyte interphase (SEI) while maintaining compatibility with aluminum (Al0) current collector. However, the intrinsic reductive mechanism through which LiDFTFSI influences battery performance remains unclear and under debate. Herein, the detailed SEI reactions of LiDFTFSI-based electrolytes were investigated by combining density functional theory and molecular dynamics, aiming to clarify the formation process and atomic structure of SEI. Our results show that asymmetric DFTFSI– weakens the interaction between carbonate solvents and Li+, and substantially alter the solvation structure, exhibiting a well-balanced coordination capacity to bis(trifluoromethanesulfonyl)imide (TFSI–). Nanoseconds hybrid molecular dynamics simulation further reveals that the preferential decomposition of LiDFTFSI produces sufficient LiF and Li2O to facilitate a robust SEI. Moreover, the abundant F– generated from LiDFTFSI decomposition accumulates on the Al surface and subsequently combines with Al3+ from the current collector to form AlF3, potentially inhibiting corrosion of the current collector. Overall, these findings elucidate how LiDFTFSI regulates the solvation sheath and SEI structure, advancing the development of high-performance electrolytes compatible with current collector.
Copyright:
This is an open access article distributed under the Creative Commons Attribution License which permits unrestricted use, distribution, and reproduction in any medium, provided the original work is properly cited.
