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Title: Atomic to Nanoscale Origin of Vinylene Carbonate Enhanced Cycling Stability of Lithium Metal Anode Revealed by Cryo-Transmission Electron Microscopy

Abstract

Batteries using lithium (Li) metal as anode are considered promising energy storage systems because of their high specific energy densities. The crucial bottlenecks for Li-metal anode are Li dendrites growth and side reactions with electrolyte inducing low Coulombic efficiency (CE) and short cycle life. Vinylene carbonate (VC), as an effective electrolyte additive in Li-ion batteries, has been noticed to significantly enhance the CE, while the origin of such an additive remains unclear. Here we use cryo-TEM imaging combing with EDS elemental and EELS electronic structure analyses to reveal the role of VC additive. We discovered that the electrochemically deposited Li metal (EDLi) in VC-containing electrolyte is slightly oxidized with the SEI being a nanoscale-mosaic like structure comprised of organic species, Li2O and Li2CO3; while the EDLi formed in VC-free electrolyte is featured by a combination of fully oxidized Li with Li2O SEI layer and pure Li metal with multilayer nano-structured SEI. These results highlight the possible tuning of crucial structural and chemical features of EDLi and SEI through additives and consequently direct correlation with electrochemical performance, providing valuable guidelines to rational selection, design and synthesis of additives for new battery chemistries.

Authors:
ORCiD logo [1]; ORCiD logo [2];  [1];  [3]; ORCiD logo [2]; ORCiD logo [2]; ORCiD logo [1]
  1. Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Environmental Molecular Sciences Lab. (EMSL)
  2. Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
  3. Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Environmental Molecular Sciences Lab. (EMSL); Chinese Academy of Sciences (CAS), Fuzhou, Fujian (People's Republic of China)
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)
OSTI Identifier:
1603103
Report Number(s):
PNNL-SA-149594
Journal ID: ISSN 1530-6984
Grant/Contract Number:  
AC05-76RL01830; AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Nano Letters
Additional Journal Information:
Journal Volume: 20; Journal Issue: 1; Journal ID: ISSN 1530-6984
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; lithium (Li) metal; cryogenic transmission electron microscopy (cryo-TEM); electrochemical deposition; solid electrolyte interphase (SEI); electrolyte; vinylene carbonate (VC)

Citation Formats

Xu, Yaobin, Wu, Haiping, He, Yang, Chen, Qingsong, Zhang, Ji-Guang, Xu, Wu, and Wang, Chongmin. Atomic to Nanoscale Origin of Vinylene Carbonate Enhanced Cycling Stability of Lithium Metal Anode Revealed by Cryo-Transmission Electron Microscopy. United States: N. p., 2019. Web. https://doi.org/10.1021/acs.nanolett.9b04111.
Xu, Yaobin, Wu, Haiping, He, Yang, Chen, Qingsong, Zhang, Ji-Guang, Xu, Wu, & Wang, Chongmin. Atomic to Nanoscale Origin of Vinylene Carbonate Enhanced Cycling Stability of Lithium Metal Anode Revealed by Cryo-Transmission Electron Microscopy. United States. https://doi.org/10.1021/acs.nanolett.9b04111
Xu, Yaobin, Wu, Haiping, He, Yang, Chen, Qingsong, Zhang, Ji-Guang, Xu, Wu, and Wang, Chongmin. Mon . "Atomic to Nanoscale Origin of Vinylene Carbonate Enhanced Cycling Stability of Lithium Metal Anode Revealed by Cryo-Transmission Electron Microscopy". United States. https://doi.org/10.1021/acs.nanolett.9b04111. https://www.osti.gov/servlets/purl/1603103.
@article{osti_1603103,
title = {Atomic to Nanoscale Origin of Vinylene Carbonate Enhanced Cycling Stability of Lithium Metal Anode Revealed by Cryo-Transmission Electron Microscopy},
author = {Xu, Yaobin and Wu, Haiping and He, Yang and Chen, Qingsong and Zhang, Ji-Guang and Xu, Wu and Wang, Chongmin},
abstractNote = {Batteries using lithium (Li) metal as anode are considered promising energy storage systems because of their high specific energy densities. The crucial bottlenecks for Li-metal anode are Li dendrites growth and side reactions with electrolyte inducing low Coulombic efficiency (CE) and short cycle life. Vinylene carbonate (VC), as an effective electrolyte additive in Li-ion batteries, has been noticed to significantly enhance the CE, while the origin of such an additive remains unclear. Here we use cryo-TEM imaging combing with EDS elemental and EELS electronic structure analyses to reveal the role of VC additive. We discovered that the electrochemically deposited Li metal (EDLi) in VC-containing electrolyte is slightly oxidized with the SEI being a nanoscale-mosaic like structure comprised of organic species, Li2O and Li2CO3; while the EDLi formed in VC-free electrolyte is featured by a combination of fully oxidized Li with Li2O SEI layer and pure Li metal with multilayer nano-structured SEI. These results highlight the possible tuning of crucial structural and chemical features of EDLi and SEI through additives and consequently direct correlation with electrochemical performance, providing valuable guidelines to rational selection, design and synthesis of additives for new battery chemistries.},
doi = {10.1021/acs.nanolett.9b04111},
journal = {Nano Letters},
number = 1,
volume = 20,
place = {United States},
year = {2019},
month = {12}
}

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