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Title: The Impact of Li Grain Size on Coulombic Efficiency in Li Batteries

Abstract

One of the most promising means to increase the energy density of state-of-the-art lithium (Li)-ion batteries is to replace the graphite anode with a Li metal anode1, 2, 3. While the direct use of Li metal may be highly advantageous4,5, at present its practical application is limited by issues related to dendrite growth and low Coulombic efficiency (CE)6. Here operando electrochemical scanning transmission electron microscopy (STEM) is used to directly image the deposition/stripping of Li at the anode-electrolyte interface in a Li-based battery. A non-aqueous electrolyte containing small amounts of H2O as an additive results in remarkably different deposition/stripping properties as compared to the "dry" electrolyte when operated under identical electrochemical conditions. The electrolyte with the additive deposits more Li during the first cycle, with the grain sizes of the Li deposits being significantly larger and more variable. Here, the stripping of the Li upon discharge is also more complete, i.e., there is a higher cycling CE. This suggests that larger grain sizes are indicative of better performance by leading to more uniform Li deposition and an overall decrease in the formation of Li dendrites and side reactions with electrolyte components, thus potentially paving the way for the direct usemore » of Li metal in battery technologies.« less

Authors:
 [1];  [1];  [1];  [2];  [1];  [1];  [1];  [3];  [4]
  1. Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
  2. Florida State Univ., Tallahassee, FL (United States)
  3. Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Pennsylvania State Univ., University Park, PA (United States)
  4. Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Univ. of Washington, Seattle, WA (United States)
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Environmental Molecular Sciences Lab. (EMSL)
Sponsoring Org.:
USDOE
OSTI Identifier:
1340836
Report Number(s):
PNNL-SA-120401
Journal ID: ISSN 2045-2322; 48681; KC0208010
Grant/Contract Number:  
AC05-76RL01830
Resource Type:
Accepted Manuscript
Journal Name:
Scientific Reports
Additional Journal Information:
Journal Volume: 6; Journal ID: ISSN 2045-2322
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; Environmental Molecular Sciences Laboratory

Citation Formats

Mehdi, B. Layla, Stevens, Andrew, Qian, Jiangfeng, Park, Chiwoo, Xu, Wu, Henderson, Wesley A., Zhang, Ji -Guang, Mueller, Karl T., and Browning, Nigel D. The Impact of Li Grain Size on Coulombic Efficiency in Li Batteries. United States: N. p., 2016. Web. doi:10.1038/srep34267.
Mehdi, B. Layla, Stevens, Andrew, Qian, Jiangfeng, Park, Chiwoo, Xu, Wu, Henderson, Wesley A., Zhang, Ji -Guang, Mueller, Karl T., & Browning, Nigel D. The Impact of Li Grain Size on Coulombic Efficiency in Li Batteries. United States. doi:10.1038/srep34267.
Mehdi, B. Layla, Stevens, Andrew, Qian, Jiangfeng, Park, Chiwoo, Xu, Wu, Henderson, Wesley A., Zhang, Ji -Guang, Mueller, Karl T., and Browning, Nigel D. Wed . "The Impact of Li Grain Size on Coulombic Efficiency in Li Batteries". United States. doi:10.1038/srep34267. https://www.osti.gov/servlets/purl/1340836.
@article{osti_1340836,
title = {The Impact of Li Grain Size on Coulombic Efficiency in Li Batteries},
author = {Mehdi, B. Layla and Stevens, Andrew and Qian, Jiangfeng and Park, Chiwoo and Xu, Wu and Henderson, Wesley A. and Zhang, Ji -Guang and Mueller, Karl T. and Browning, Nigel D.},
abstractNote = {One of the most promising means to increase the energy density of state-of-the-art lithium (Li)-ion batteries is to replace the graphite anode with a Li metal anode1, 2, 3. While the direct use of Li metal may be highly advantageous4,5, at present its practical application is limited by issues related to dendrite growth and low Coulombic efficiency (CE)6. Here operando electrochemical scanning transmission electron microscopy (STEM) is used to directly image the deposition/stripping of Li at the anode-electrolyte interface in a Li-based battery. A non-aqueous electrolyte containing small amounts of H2O as an additive results in remarkably different deposition/stripping properties as compared to the "dry" electrolyte when operated under identical electrochemical conditions. The electrolyte with the additive deposits more Li during the first cycle, with the grain sizes of the Li deposits being significantly larger and more variable. Here, the stripping of the Li upon discharge is also more complete, i.e., there is a higher cycling CE. This suggests that larger grain sizes are indicative of better performance by leading to more uniform Li deposition and an overall decrease in the formation of Li dendrites and side reactions with electrolyte components, thus potentially paving the way for the direct use of Li metal in battery technologies.},
doi = {10.1038/srep34267},
journal = {Scientific Reports},
number = ,
volume = 6,
place = {United States},
year = {2016},
month = {10}
}

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