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Current Density Regulated Atomic to Nanoscale Process on Li Deposition and Solid Electrolyte Interphase Revealed by Cryogenic Transmission Electron Microscopy.
ACS Nano. 2020 Jul 06 [Online ahead of print]AN

Abstract

Current density has been perceived to play a critical rule in controlling Li deposition morphology and solid electrolyte interphase (SEI). However, the atomic level mechanism of the effect of current density on Li deposition and the SEI remains unclear. Here based on cryogenic transmission electron microscopy (TEM) imaging combined with energy dispersive X-ray spectroscopy (EDS) and electron energy loss spectroscopy (EELS) electronic structure analyses, we reveal the atomic level correlation of Li deposition morphology and SEI with current density. We discover that increasing current density leads to increased overpotential for Li nucleation and growth, leading to the transition from growth-limited to nucleation-limited mode for Li dendrites. Independent of current density, the electrochemically deposited Li metal (EDLi) exhibits crystalline whisker-like morphology. The SEI formed at low current density (0.1 mA cm-2) is monolithic amorphous; while, a current density of above 2 mA cm-2 leads to a mosaic structured SEI, featuring an amorphous matrix with Li2O and LiF dispersoids, and the thickness of the SEI increases with the increase of current density. Specifically, the Li2O particles are spatially located at the top surface of the SEI, while LiF is spatially adjacent to the Li-SEI interface. These results offer possible ways of regulating crucial microstructural and chemical features of EDLi and SEI through altering deposit conditions and consequently direct correlation with battery performance.

Authors+Show Affiliations

Environmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory, Richland, Washington 99354, United States.Energy and Environment Directorate, Pacific Northwest National Laboratory, Richland, Washington 99354, United States.Energy and Environment Directorate, Pacific Northwest National Laboratory, Richland, Washington 99354, United States.Energy and Environment Directorate, Pacific Northwest National Laboratory, Richland, Washington 99354, United States.Energy and Environment Directorate, Pacific Northwest National Laboratory, Richland, Washington 99354, United States.Environmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory, Richland, Washington 99354, United States.

Pub Type(s)

Journal Article

Language

eng

PubMed ID

32598126

Citation

Xu, Yaobin, et al. "Current Density Regulated Atomic to Nanoscale Process On Li Deposition and Solid Electrolyte Interphase Revealed By Cryogenic Transmission Electron Microscopy." ACS Nano, 2020.
Xu Y, Wu H, Jia H, et al. Current Density Regulated Atomic to Nanoscale Process on Li Deposition and Solid Electrolyte Interphase Revealed by Cryogenic Transmission Electron Microscopy. ACS Nano. 2020.
Xu, Y., Wu, H., Jia, H., Zhang, J. G., Xu, W., & Wang, C. (2020). Current Density Regulated Atomic to Nanoscale Process on Li Deposition and Solid Electrolyte Interphase Revealed by Cryogenic Transmission Electron Microscopy. ACS Nano. https://doi.org/10.1021/acsnano.0c03344
Xu Y, et al. Current Density Regulated Atomic to Nanoscale Process On Li Deposition and Solid Electrolyte Interphase Revealed By Cryogenic Transmission Electron Microscopy. ACS Nano. 2020 Jul 6; PubMed PMID: 32598126.
* Article titles in AMA citation format should be in sentence-case
TY - JOUR T1 - Current Density Regulated Atomic to Nanoscale Process on Li Deposition and Solid Electrolyte Interphase Revealed by Cryogenic Transmission Electron Microscopy. AU - Xu,Yaobin, AU - Wu,Haiping, AU - Jia,Hao, AU - Zhang,Ji-Guang, AU - Xu,Wu, AU - Wang,Chongmin, Y1 - 2020/07/06/ PY - 2020/7/1/pubmed PY - 2020/7/1/medline PY - 2020/6/30/entrez KW - Li metal KW - cryo-TEM KW - current density KW - electrochemical deposition KW - microstructure KW - solid electrolyte interphase JF - ACS nano JO - ACS Nano N2 - Current density has been perceived to play a critical rule in controlling Li deposition morphology and solid electrolyte interphase (SEI). However, the atomic level mechanism of the effect of current density on Li deposition and the SEI remains unclear. Here based on cryogenic transmission electron microscopy (TEM) imaging combined with energy dispersive X-ray spectroscopy (EDS) and electron energy loss spectroscopy (EELS) electronic structure analyses, we reveal the atomic level correlation of Li deposition morphology and SEI with current density. We discover that increasing current density leads to increased overpotential for Li nucleation and growth, leading to the transition from growth-limited to nucleation-limited mode for Li dendrites. Independent of current density, the electrochemically deposited Li metal (EDLi) exhibits crystalline whisker-like morphology. The SEI formed at low current density (0.1 mA cm-2) is monolithic amorphous; while, a current density of above 2 mA cm-2 leads to a mosaic structured SEI, featuring an amorphous matrix with Li2O and LiF dispersoids, and the thickness of the SEI increases with the increase of current density. Specifically, the Li2O particles are spatially located at the top surface of the SEI, while LiF is spatially adjacent to the Li-SEI interface. These results offer possible ways of regulating crucial microstructural and chemical features of EDLi and SEI through altering deposit conditions and consequently direct correlation with battery performance. SN - 1936-086X UR - https://www.unboundmedicine.com/medline/citation/32598126/Current_Density_Regulated_Atomic_to_Nanoscale_Process_on_Li_Deposition_and_Solid_Electrolyte_Interphase_Revealed_by_Cryogenic_Transmission_Electron_Microscopy L2 - https://doi.org/10.1021/acsnano.0c03344 DB - PRIME DP - Unbound Medicine ER -
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