Evolution and interplay of lithium metal interphase components revealed by experimental and theoretical studies

Tan, Sha; Kuai, Dacheng; Yu, Zhiao; Beltran, Saul P.; Rahman, Muhammad M.; 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 May 01 04:00:00 EDT 2024 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.3c14232· OSTI ID:2440494

Tan, Sha ^[1]; Kuai, Dacheng ^[2]; Yu, Zhiao ^[3]; Beltran, Saul P. ^[2]; Rahman, Muhammad M. ^[1]; Xia, Kangxuan ^[1]; Wang, Nan ^[1]; Chen, Yuelang ^[3]; Yang, Xiao-Qing ^[1]; Xiao, Jie ^[4]; Liu, Jun ^[5]; Cui, Yi ^[3]; Bao, Zhenan ^[3]; Balbuena, Perla B. ^[2]; Hu, Enyuan ^[1]

Brookhaven National Laboratory
Texas A & M University
Stanford University
BATTELLE (PACIFIC NW LAB)
PNNL

ABSTRACT: 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 quantitative-ly with statistical significance, we study the composition and dynamics of LMB interphase for a newly developed im-portant 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.

Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: USDOE

DOE Contract Number:: AC05-76RL01830

OSTI ID:: 2440494

Report Number(s):: PNNL-SA-197510

Journal Information:: Journal of the American Chemical Society, Journal Name: Journal of the American Chemical Society Journal Issue: 17 Vol. 146

Country of Publication:: United States

Language:: English

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