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Title: Detrimental Effects of Chemical Crossover from the Lithium Anode to Cathode in Rechargeable Lithium Metal Batteries

Abstract

The interfacial stability is one of the crucial factors affecting long-term cyclability of lithium (Li) metal batteries (LMBs). While cross contamination (such as Mn+2 crossover from cathode to contaminate graphite anode) phenomena has been well studied in Li ion batteries (LIBs), the similar phenomena has rarely been studied in LMBs. Here, we systematically investigated the cathode failure triggered by the chemical crossover between the electrode pair in rechargeable LMBs. In strong contrast to LIBs, the cathode in LMBs suffers more significant and irreversible capacity fade during cycling and its capacity cannot be fully recovered even when Li metal anode has been replaced in the successive cycling. In-depth characterizations of the cathode surface reveal severe CEI deterioration related to the accumulation of highly resistive polymeric components and lithium fluoride. The soluble decomposition products generated by extensive salt-anion decomposition at Li metal surface can diffuse toward cathode side and result in severe deterioration of cathode as well asseparator surfaces. A polydopamine coated separator with selective Li-ion permeability has been developed to mitigate the detrimental chemical crossover and enhance the cathode stability.

Authors:
ORCiD logo [1];  [1];  [1];  [1]; ORCiD logo [2]; ORCiD logo [2];  [3]; ORCiD logo [3];  [4]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]
  1. Energy &, Environment Directorate, Pacific Northwest National Laboratory (PNNL), 902 Battelle Boulevard, Richland, Washington 99354, United States
  2. Environmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory (PNNL), 3335 Innovation Boulevard, Richland, Washington 99354, United States
  3. Department of Chemical &, Biomolecular Engineering, Korea Advanced Institute of Science and Technology (KAIST), 291 Daehak-ro, Yuseong-gu, Daejeon 34141, Republic of Korea
  4. Energy &, Environment Directorate, Pacific Northwest National Laboratory (PNNL), 902 Battelle Boulevard, Richland, Washington 99354, United States; Department of Chemistry &, Biochemistry, University of Arkansas, Fayetteville, Arkansas 72701, United States
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)
OSTI Identifier:
1496565
Report Number(s):
PNNL-SA-137789
Journal ID: ISSN 2380-8195
DOE Contract Number:  
AC05-76RL01830
Resource Type:
Journal Article
Journal Name:
ACS Energy Letters
Additional Journal Information:
Journal Volume: 3; Journal Issue: 12; Journal ID: ISSN 2380-8195
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English

Citation Formats

Lee, Hongkyung, Lim, Hyung-Seok, Ren, Xiaodi, Yu, Lu, Engelhard, Mark H., Han, Kee Sung, Lee, Jinhong, Kim, Hee-Tak, Xiao, Jie, Liu, Jun, Xu, Wu, and Zhang, Ji-Guang. Detrimental Effects of Chemical Crossover from the Lithium Anode to Cathode in Rechargeable Lithium Metal Batteries. United States: N. p., 2018. Web. doi:10.1021/acsenergylett.8b01819.
Lee, Hongkyung, Lim, Hyung-Seok, Ren, Xiaodi, Yu, Lu, Engelhard, Mark H., Han, Kee Sung, Lee, Jinhong, Kim, Hee-Tak, Xiao, Jie, Liu, Jun, Xu, Wu, & Zhang, Ji-Guang. Detrimental Effects of Chemical Crossover from the Lithium Anode to Cathode in Rechargeable Lithium Metal Batteries. United States. doi:10.1021/acsenergylett.8b01819.
Lee, Hongkyung, Lim, Hyung-Seok, Ren, Xiaodi, Yu, Lu, Engelhard, Mark H., Han, Kee Sung, Lee, Jinhong, Kim, Hee-Tak, Xiao, Jie, Liu, Jun, Xu, Wu, and Zhang, Ji-Guang. Fri . "Detrimental Effects of Chemical Crossover from the Lithium Anode to Cathode in Rechargeable Lithium Metal Batteries". United States. doi:10.1021/acsenergylett.8b01819.
@article{osti_1496565,
title = {Detrimental Effects of Chemical Crossover from the Lithium Anode to Cathode in Rechargeable Lithium Metal Batteries},
author = {Lee, Hongkyung and Lim, Hyung-Seok and Ren, Xiaodi and Yu, Lu and Engelhard, Mark H. and Han, Kee Sung and Lee, Jinhong and Kim, Hee-Tak and Xiao, Jie and Liu, Jun and Xu, Wu and Zhang, Ji-Guang},
abstractNote = {The interfacial stability is one of the crucial factors affecting long-term cyclability of lithium (Li) metal batteries (LMBs). While cross contamination (such as Mn+2 crossover from cathode to contaminate graphite anode) phenomena has been well studied in Li ion batteries (LIBs), the similar phenomena has rarely been studied in LMBs. Here, we systematically investigated the cathode failure triggered by the chemical crossover between the electrode pair in rechargeable LMBs. In strong contrast to LIBs, the cathode in LMBs suffers more significant and irreversible capacity fade during cycling and its capacity cannot be fully recovered even when Li metal anode has been replaced in the successive cycling. In-depth characterizations of the cathode surface reveal severe CEI deterioration related to the accumulation of highly resistive polymeric components and lithium fluoride. The soluble decomposition products generated by extensive salt-anion decomposition at Li metal surface can diffuse toward cathode side and result in severe deterioration of cathode as well asseparator surfaces. A polydopamine coated separator with selective Li-ion permeability has been developed to mitigate the detrimental chemical crossover and enhance the cathode stability.},
doi = {10.1021/acsenergylett.8b01819},
journal = {ACS Energy Letters},
issn = {2380-8195},
number = 12,
volume = 3,
place = {United States},
year = {2018},
month = {11}
}