Nucleation and Early Stage Growth of Li Electrodeposits
Abstract
The morphologies metal electrodeposits adopt during the earliest stages of electrodeposition are known to play a critical role in the recharge of electrochemical cells that use metals as anodes. In this work, we report results from a combined theoretical and experimental study of the early-stage nucleation and growth of electrodeposited lithium at liquid-solid interfaces. The spatial characteristics of Lithium electrodeposits are studied via Scanning Electron Microscopy in tandem with Image analysis. Comparisons of Li nucleation and growth in multiple electrolytes provide a comprehensive picture of the initial nucleation and growth dynamics. We report that ion diffusion in the bulk electrolyte and through the Solid Electrolyte Interphase (SEI) formed spontaneously on the metal play equally important roles on Li nucleation and growth. Furthermore, we postulate that the underlying physics dictating bulk and surface diffusion are similar across a range of electrolyte chemistries and measurement conditions and that fluorinated electrolytes produce a distinct flattening of Li electrodeposits at low rates. These observations are rationalized using X-ray Photoelectron Spectroscopy (XPS), Electrochemical Impedance Spectroscopy (EIS), and contact angle goniometry to probe the interfacial chemistry and dynamics. Our results show that high interfacial energy and high surface ion diffusivity are necessary for uniform Li plating.
- Authors:
-
- Cornell Univ., Ithaca, NY (United States). Robert Frederick Smith School of Chemical and Biomolecular Engineering
- Stanford Univ., CA (United States). Dept. of Chemical Engineering
- Publication Date:
- Research Org.:
- Energy Frontier Research Centers (EFRC) (United States). Center for Mesoscale Transport Properties (m2mt); Stony Brook Univ., NY (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)
- OSTI Identifier:
- 1597278
- Grant/Contract Number:
- SC0012673; DMR-1719875
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Nano Letters
- Additional Journal Information:
- Journal Volume: 19; Journal Issue: 11; Journal ID: ISSN 1530-6984
- Publisher:
- American Chemical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 25 ENERGY STORAGE; Lithium metal anode; nucleation and growth; surface ion diffusion; interfacial energy
Citation Formats
Biswal, Prayag, Stalin, Sanjuna, Kludze, Atsu, Choudhury, Snehashis, and Archer, Lynden A. Nucleation and Early Stage Growth of Li Electrodeposits. United States: N. p., 2019.
Web. doi:10.1021/acs.nanolett.9b03548.
Biswal, Prayag, Stalin, Sanjuna, Kludze, Atsu, Choudhury, Snehashis, & Archer, Lynden A. Nucleation and Early Stage Growth of Li Electrodeposits. United States. https://doi.org/10.1021/acs.nanolett.9b03548
Biswal, Prayag, Stalin, Sanjuna, Kludze, Atsu, Choudhury, Snehashis, and Archer, Lynden A. Mon .
"Nucleation and Early Stage Growth of Li Electrodeposits". United States. https://doi.org/10.1021/acs.nanolett.9b03548. https://www.osti.gov/servlets/purl/1597278.
@article{osti_1597278,
title = {Nucleation and Early Stage Growth of Li Electrodeposits},
author = {Biswal, Prayag and Stalin, Sanjuna and Kludze, Atsu and Choudhury, Snehashis and Archer, Lynden A.},
abstractNote = {The morphologies metal electrodeposits adopt during the earliest stages of electrodeposition are known to play a critical role in the recharge of electrochemical cells that use metals as anodes. In this work, we report results from a combined theoretical and experimental study of the early-stage nucleation and growth of electrodeposited lithium at liquid-solid interfaces. The spatial characteristics of Lithium electrodeposits are studied via Scanning Electron Microscopy in tandem with Image analysis. Comparisons of Li nucleation and growth in multiple electrolytes provide a comprehensive picture of the initial nucleation and growth dynamics. We report that ion diffusion in the bulk electrolyte and through the Solid Electrolyte Interphase (SEI) formed spontaneously on the metal play equally important roles on Li nucleation and growth. Furthermore, we postulate that the underlying physics dictating bulk and surface diffusion are similar across a range of electrolyte chemistries and measurement conditions and that fluorinated electrolytes produce a distinct flattening of Li electrodeposits at low rates. These observations are rationalized using X-ray Photoelectron Spectroscopy (XPS), Electrochemical Impedance Spectroscopy (EIS), and contact angle goniometry to probe the interfacial chemistry and dynamics. Our results show that high interfacial energy and high surface ion diffusivity are necessary for uniform Li plating.},
doi = {10.1021/acs.nanolett.9b03548},
journal = {Nano Letters},
number = 11,
volume = 19,
place = {United States},
year = {Mon Sep 30 00:00:00 EDT 2019},
month = {Mon Sep 30 00:00:00 EDT 2019}
}
Web of Science
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Works referencing / citing this record:
A Sustainable Solid Electrolyte Interphase for High‐Energy‐Density Lithium Metal Batteries Under Practical Conditions
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A Sustainable Solid Electrolyte Interphase for High‐Energy‐Density Lithium Metal Batteries Under Practical Conditions
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Inside Back Cover: A Sustainable Solid Electrolyte Interphase for High‐Energy‐Density Lithium Metal Batteries Under Practical Conditions (Angew. Chem. Int. Ed. 8/2020)
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