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Solvation Structure Engineering of Weakly Coordinating Sulfonamide Electrolytes for 4.6 V Lithium Metal Batteries

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Authors

Pompizii, Lea; Liu, Mingliang; Braks, Leonie; Ashirov, Timur; Zhou, Tianhong; Mensi, Mounir; Park, Dongmin; Choi, Jang Wook; Coskun, Ali

Issue Date
2024-12
Publisher
American Chemical Society
Citation
ACS Energy Letters, Vol.10 No.1, pp.246-253
Abstract
A series of trifluoromethanesulfonamide solvents were synthesized with systematically controlled ring size (4-6) at the N-terminal to tune their steric and electronic properties to realize enhanced contact ion pairs for the formation of an anion-derived solid-electrolyte interface (SEI) and compatibility with the NMC811 cathode. Comparative analyses of electrolytes revealed that the 1.6 M LiFSI 1-azetidine trifluoromethanesulfonamide (AzTFSA) electrolyte presents the ideal combination of steric and electronic effects along with high oxidation stability up to 5 V and a Coulombic efficiency of 99.2% in Cu-Li half-cells at 1 mA cm-2 and 1 mAh cm-2. The corresponding full cells using 20 mu m of Li foil paired with the NCM811 cathode by a negative and positive capacity ratio (N/P) of 2.5, achieve 80% capacity retention after 150 cycles at 0.5C. Even at a high charge cutoff voltage of 4.6 V, the Li|NCM811 full cell still realizes 92% retention at 0.5C after 100 cycles.
URI
https://hdl.handle.net/10371/216418
DOI
https://doi.org/10.1021/acsenergylett.4c03030
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  • College of Engineering
  • School of Chemical and Biological Engineering
Research Area Physics, Materials Science

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