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Title: Electrode Edge Effects and the Failure Mechanism of Lithium-Metal Batteries

Abstract

Lithium (Li) metal with very high specific capacity makes it one of the ideal anode for high energy batteries. However, Li dendrite growth and the formation of isolated (or “dead”) Li during repeated Li plating/stripping processes lead to its low Coulombic efficiency (CE). In this work, we discovered for the first time that part of Li CE loss can be attributed to the edge effect of the copper (Cu) substrate electrode in a conventional Li||Cu cell configuration. The “dead” Li formed on the edge of Cu substrate was systematically investigated through scanning electron microscopy, energy dispersive X-ray spectroscopy, and two-dimensional X-ray photoelectron spectroscopy. In order to minimize the Li loss at the edge of the Cu exposed to pressure-free space, modified Li||Cu cell configuration with a Cu electrode smaller than Li metal is preferred. It was clearly demonstrated that using an electrode configuration with minimal open space or “pressure-free space” across electrodes can reduce “dead” Li accumulated during cycling and increase Li CE. This phenomena was also verified in Li metal batteries (Li||LiNi1/3Mn1/3Co1/3O2) and should be considered in the design of practical Li metal batteries.

Authors:
ORCiD logo [1];  [1];  [1];  [2];  [2];  [2];  [2];  [1];  [1];  [1]; ORCiD logo [1]
  1. Energy and Environment Directorate, Pacific Northwest National Laboratory, 902 Battelle Boulevard. Richland Washington 99354 USA
  2. Environmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory, 3335 Innovation Boulevard Richland Washington 99354 USA
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V); USDOE Office of Science (SC), Biological and Environmental Research (BER) (SC-23)
OSTI Identifier:
1492555
Report Number(s):
PNNL-SA-134550
Journal ID: ISSN 1864-5631
DOE Contract Number:  
AC05-76RL01830
Resource Type:
Journal Article
Journal Name:
ChemSusChem
Additional Journal Information:
Journal Volume: 11; Journal Issue: 21; Journal ID: ISSN 1864-5631
Publisher:
ChemPubSoc Europe
Country of Publication:
United States
Language:
English

Citation Formats

Lee, Hongkyung, Chen, Shuru, Ren, Xiaodi, Martinez, Abraham, Shutthanandan, Vaithiyalingam, Vijayakumar, Murugesan, Han, Kee Sung, Li, Qiuyan, Liu, Jun, Xu, Wu, and Zhang, Ji-Guang. Electrode Edge Effects and the Failure Mechanism of Lithium-Metal Batteries. United States: N. p., 2018. Web. doi:10.1002/cssc.201801445.
Lee, Hongkyung, Chen, Shuru, Ren, Xiaodi, Martinez, Abraham, Shutthanandan, Vaithiyalingam, Vijayakumar, Murugesan, Han, Kee Sung, Li, Qiuyan, Liu, Jun, Xu, Wu, & Zhang, Ji-Guang. Electrode Edge Effects and the Failure Mechanism of Lithium-Metal Batteries. United States. doi:10.1002/cssc.201801445.
Lee, Hongkyung, Chen, Shuru, Ren, Xiaodi, Martinez, Abraham, Shutthanandan, Vaithiyalingam, Vijayakumar, Murugesan, Han, Kee Sung, Li, Qiuyan, Liu, Jun, Xu, Wu, and Zhang, Ji-Guang. Thu . "Electrode Edge Effects and the Failure Mechanism of Lithium-Metal Batteries". United States. doi:10.1002/cssc.201801445.
@article{osti_1492555,
title = {Electrode Edge Effects and the Failure Mechanism of Lithium-Metal Batteries},
author = {Lee, Hongkyung and Chen, Shuru and Ren, Xiaodi and Martinez, Abraham and Shutthanandan, Vaithiyalingam and Vijayakumar, Murugesan and Han, Kee Sung and Li, Qiuyan and Liu, Jun and Xu, Wu and Zhang, Ji-Guang},
abstractNote = {Lithium (Li) metal with very high specific capacity makes it one of the ideal anode for high energy batteries. However, Li dendrite growth and the formation of isolated (or “dead”) Li during repeated Li plating/stripping processes lead to its low Coulombic efficiency (CE). In this work, we discovered for the first time that part of Li CE loss can be attributed to the edge effect of the copper (Cu) substrate electrode in a conventional Li||Cu cell configuration. The “dead” Li formed on the edge of Cu substrate was systematically investigated through scanning electron microscopy, energy dispersive X-ray spectroscopy, and two-dimensional X-ray photoelectron spectroscopy. In order to minimize the Li loss at the edge of the Cu exposed to pressure-free space, modified Li||Cu cell configuration with a Cu electrode smaller than Li metal is preferred. It was clearly demonstrated that using an electrode configuration with minimal open space or “pressure-free space” across electrodes can reduce “dead” Li accumulated during cycling and increase Li CE. This phenomena was also verified in Li metal batteries (Li||LiNi1/3Mn1/3Co1/3O2) and should be considered in the design of practical Li metal batteries.},
doi = {10.1002/cssc.201801445},
journal = {ChemSusChem},
issn = {1864-5631},
number = 21,
volume = 11,
place = {United States},
year = {2018},
month = {10}
}