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Title: Lithium electrodeposition dynamics in aprotic electrolyte observed in situ via transmission electron microscopy

Abstract

Electrodeposited metallic lithium is an ideal negative battery electrode, but nonuniform microstructure evolution during cycling leads to degradation and safety issues. A better understanding of the Li plating and stripping processes is needed to enable practical Li-metal batteries. Here we use a custom microfabricated, sealed liquid cell for in situ scanning transmission electron microscopy (STEM) to image the first few cycles of lithium electrodeposition/dissolution in liquid aprotic electrolyte at submicron resolution. Cycling at current densities from 1 to 25 mA/cm 2 leads to variations in grain structure, with higher current densities giving a more needle-like, higher surface area deposit. The effect of the electron beam was explored, and it was found that, even with minimal beam exposure, beam-induced surface film formation could alter the Li microstructure. The electrochemical dissolution was seen to initiate from isolated points on grains rather than uniformly across the Li surface, due to the stabilizing solid electrolyte interphase surface film. As a result, we discuss the implications for operando STEM liquid-cell imaging and Li-battery applications.

Authors:
 [1];  [1];  [1];  [1];  [1]
  1. Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
Publication Date:
Research Org.:
Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1235316
Report Number(s):
SAND-2015-2431J
Journal ID: ISSN 1936-0851; 579677
Grant/Contract Number:
AC04-94AL85000
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
ACS Nano
Additional Journal Information:
Journal Volume: 9; Journal Issue: 4; Journal ID: ISSN 1936-0851
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
lithium electrodeposition; liquid-cell electron microscopy; electron beam radiolysis; lithium-ion battery; solid electrolyte interphase; in situ TEM

Citation Formats

Leenheer, Andrew Jay, Jungjohann, Katherine Leigh, Zavadil, Kevin Robert, Sullivan, John P., and Harris, Charles Thomas. Lithium electrodeposition dynamics in aprotic electrolyte observed in situ via transmission electron microscopy. United States: N. p., 2015. Web. doi:10.1021/acsnano.5b00876.
Leenheer, Andrew Jay, Jungjohann, Katherine Leigh, Zavadil, Kevin Robert, Sullivan, John P., & Harris, Charles Thomas. Lithium electrodeposition dynamics in aprotic electrolyte observed in situ via transmission electron microscopy. United States. doi:10.1021/acsnano.5b00876.
Leenheer, Andrew Jay, Jungjohann, Katherine Leigh, Zavadil, Kevin Robert, Sullivan, John P., and Harris, Charles Thomas. Wed . "Lithium electrodeposition dynamics in aprotic electrolyte observed in situ via transmission electron microscopy". United States. doi:10.1021/acsnano.5b00876. https://www.osti.gov/servlets/purl/1235316.
@article{osti_1235316,
title = {Lithium electrodeposition dynamics in aprotic electrolyte observed in situ via transmission electron microscopy},
author = {Leenheer, Andrew Jay and Jungjohann, Katherine Leigh and Zavadil, Kevin Robert and Sullivan, John P. and Harris, Charles Thomas},
abstractNote = {Electrodeposited metallic lithium is an ideal negative battery electrode, but nonuniform microstructure evolution during cycling leads to degradation and safety issues. A better understanding of the Li plating and stripping processes is needed to enable practical Li-metal batteries. Here we use a custom microfabricated, sealed liquid cell for in situ scanning transmission electron microscopy (STEM) to image the first few cycles of lithium electrodeposition/dissolution in liquid aprotic electrolyte at submicron resolution. Cycling at current densities from 1 to 25 mA/cm2 leads to variations in grain structure, with higher current densities giving a more needle-like, higher surface area deposit. The effect of the electron beam was explored, and it was found that, even with minimal beam exposure, beam-induced surface film formation could alter the Li microstructure. The electrochemical dissolution was seen to initiate from isolated points on grains rather than uniformly across the Li surface, due to the stabilizing solid electrolyte interphase surface film. As a result, we discuss the implications for operando STEM liquid-cell imaging and Li-battery applications.},
doi = {10.1021/acsnano.5b00876},
journal = {ACS Nano},
number = 4,
volume = 9,
place = {United States},
year = {Wed Mar 18 00:00:00 EDT 2015},
month = {Wed Mar 18 00:00:00 EDT 2015}
}

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Cited by: 31 works
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