Evolution and Interplay of Lithium Metal Interphase Components Revealed by Experimental and Theoretical Studies

Tan, Sha; Kuai, Dacheng; Yu, Zhiao; Perez-Beltran, Saul; Rahman, Muhammad Mominur; Xia, Kangxuan; Wang, Nan; Chen, Yuelang; Yang, Xiao-Qing; Xiao, Jie; Liu, Jun; Cui, Yi; Bao, Zhenan; Balbuena, Perla B.; Hu, Enyuan

doi:10.1021/jacs.3c14232

Evolution and Interplay of Lithium Metal Interphase Components Revealed by Experimental and Theoretical Studies

Journal Article · Wed Apr 17 00:00:00 EDT 2024 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.3c14232· OSTI ID:2340728

^[1]; Kuai, Dacheng ^[2]; ^[3]; Perez-Beltran, Saul ^[2]; Rahman, Muhammad Mominur ^[1]; Xia, Kangxuan ^[1]; ^[1]; ^[3]; ^[1]; ^[4]; ^[4]; ^[5]; ^[3]; ^[2]; ^[1]

Brookhaven National Laboratory (BNL), Upton, NY (United States)
Texas A & M Univ., College Station, TX (United States)
Stanford Univ., CA (United States)
Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
Stanford Univ., CA (United States); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). Stanford Institute for Materials and Energy Science (SIMES)

Lithium metal batteries (LMB) have high energy densities and are crucial for clean energy solutions. The characterization of lithium metal interphase is fundamentally and practically important but technically challenging. Taking advantage of synchrotron x-ray which has the unique capability of analyzing crystalline/amorphous phases quantitatively with statistical significance, here we study the composition and dynamics of LMB interphase for a newly developed important LMB electrolyte that is based on fluorinated ether. Pair distribution function analysis revealed the sequential role of anion and solvent in interphase formation during cycling. The relative ratio between Li₂O and LiF first increases and then decreases during cycling, suggesting suppressed Li₂O formation in both initial and long extended cycles. Theoretical studies revealed that in initial cycles, this is due to the energy barrier in many-electron transfer. In long extended cycles, the anion decomposition product Li₂O encourages solvent decomposition by facilitating solvent adsorption on Li₂O which is followed by concurrent depletion of both. This work highlights the important role of Li₂O in transitioning from anion-derived interphase to a solvent-derived one.

View Accepted Manuscript (DOE)

Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States); Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Vehicle Technologies Office (VTO)

Grant/Contract Number:: AC05-76RL01830; SC0012704

OSTI ID:: 2340728

Alternate ID(s):: OSTI ID: 2440494

Report Number(s):: BNL--225553-2024-JAAM

Journal Information:: Journal of the American Chemical Society, Journal Name: Journal of the American Chemical Society Journal Issue: 17 Vol. 146; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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