Lithium Electrodeposition Dynamics in Aprotic Electrolyte Observed in Situ via Transmission Electron Microscopy

ACS Nano
Andrew J LeenheerC Thomas Harris

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. We discuss the implications for operando STEM liquid-cell imaging and Li-battery applications.

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Citations

Dec 3, 2015·Analytical Chemistry·Stephen M OjaBo Zhang
Mar 30, 2016·Chemical Society Reviews·Qi ZhangTianyou Zhai
May 5, 2016·Microscopy Research and Technique·Mohammed Hammad FaweyChristian Kübel
May 25, 2016·Annual Review of Physical Chemistry·Hong-Gang Liao, Haimei Zheng
Mar 8, 2017·Nature Nanotechnology·Dingchang LinYi Cui
Jun 7, 2017·Advanced Materials·Yanpeng GuoTianyou Zhai
Dec 21, 2017·Nature Communications·Nicholas M SchneiderFrances M Ross
Jun 3, 2018·Nature Communications·Shasha LvMarnix Wagemaker
Jan 9, 2018·Chemical Society Reviews·Alok M TripathiBing Joe Hwang
Jun 10, 2021·Nano Letters·Hongyi PanHong Li
May 8, 2019·Journal of the American Chemical Society·Seung-Ho YuHéctor D Abruña

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