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

Leenheer, Andrew Jay; Jungjohann, Katherine Leigh; Zavadil, Kevin Robert; Sullivan, John P.; Harris, Charles Thomas

doi:10.1021/acsnano.5b00876

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

Journal Article · Wed Mar 18 00:00:00 EDT 2015 · ACS Nano

DOI:https://doi.org/10.1021/acsnano.5b00876· OSTI ID:1235316

Leenheer, Andrew Jay ^[1]; Jungjohann, Katherine Leigh ^[1]; Zavadil, Kevin Robert ^[1]; Sullivan, John P. ^[1]; Harris, Charles Thomas ^[1]

Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)

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.

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Research Organization:: Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC04-94AL85000

OSTI ID:: 1235316

Report Number(s):: SAND-2015-2431J; 579677

Journal Information:: ACS Nano, Vol. 9, Issue 4; ISSN 1936-0851

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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

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