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Title: Pristine or Highly Defective? Understanding the Role of Graphene Structure for Stable Lithium Metal Plating

Abstract

Abstract The role of graphene host structure/chemistry in plating–stripping in lithium metal anodes employed for lithium metal batteries is first examined in this study. Structural and chemical defects are bad, since highly defective graphene promotes unstable solid electrolyte interphase (SEI) growth. This consumes the fluoroethylene carbonate (FEC) additive in the carbonate electrolyte and is correlated with rapid decay in Coulombic efficiency (CE) and formation of filament‐like Li dendrites. A unique flow‐aided sonication exfoliation method is employed to synthesize “defect‐free” graphene (df‐G), allowing for a direct performance comparison with conventional reduced graphene oxide (r‐GO). At cycle 1, the r‐GO is better electrochemically wetted by Li than df‐G, indicating that initially it is more lithiophilic. With cycling, the nucleation overpotential with r‐GO becomes higher than with df‐G, indicating less facile plating reactions. The df‐G yields state‐of‐the‐art electrochemical performance, with the post cycled metal surface being relatively smooth and dendrite‐free. Conversely, r‐GO templates have CE rapidly degrade from the onset, with extensive dendrites after cycling. Severe SEI growth and associated FEC depletion with r‐GO are further confirmed by electrochemical impedance analysis and surface science methods. A new design rule is provided for Li metal templates: An ideal host must be noncatalytic toward SEImore » formation.« less

Authors:
ORCiD logo [1];  [1];  [1];  [1];  [1];  [2];  [3]; ORCiD logo [4]
  1. Sichuan Univ., Chengdu (China). Inst. of New-Energy and Low-Carbon Technology
  2. Sichuan Univ., Chengdu (China). Inst. of New-Energy and Low-Carbon Technology; Sichuan Univ., Chengdu (China)
  3. Clarkson Univ., Potsdam, NY (United States)
  4. Sichuan Univ., Chengdu (China). Inst. of New-Energy and Low-Carbon Technology; Clarkson Univ., Potsdam, NY (United States)
Publication Date:
Research Org.:
Clarkson Univ., Potsdam, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division; National Natural Science Foundation of China (NSFC); China Postdoctoral Science Foundation; USDOE
OSTI Identifier:
1612832
Alternate Identifier(s):
OSTI ID: 1483440
Grant/Contract Number:  
SC0018074; 51702223; 2017M623028; DE‐SC0018074
Resource Type:
Accepted Manuscript
Journal Name:
Advanced Energy Materials
Additional Journal Information:
Journal Volume: 9; Journal Issue: 3; Journal ID: ISSN 1614-6832
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; liquid phase exfoliation (LPE); mossy dendrites; sodium metal batteries (SMB); solid electrolyte interfaces (SEI)

Citation Formats

Liu, Wei, Xia, Yuting, Wang, Wenwu, Wang, Yizhe, Jin, Jialun, Chen, Yungui, Paek, Eunsu, and Mitlin, David. Pristine or Highly Defective? Understanding the Role of Graphene Structure for Stable Lithium Metal Plating. United States: N. p., 2018. Web. doi:10.1002/aenm.201802918.
Liu, Wei, Xia, Yuting, Wang, Wenwu, Wang, Yizhe, Jin, Jialun, Chen, Yungui, Paek, Eunsu, & Mitlin, David. Pristine or Highly Defective? Understanding the Role of Graphene Structure for Stable Lithium Metal Plating. United States. https://doi.org/10.1002/aenm.201802918
Liu, Wei, Xia, Yuting, Wang, Wenwu, Wang, Yizhe, Jin, Jialun, Chen, Yungui, Paek, Eunsu, and Mitlin, David. Tue . "Pristine or Highly Defective? Understanding the Role of Graphene Structure for Stable Lithium Metal Plating". United States. https://doi.org/10.1002/aenm.201802918. https://www.osti.gov/servlets/purl/1612832.
@article{osti_1612832,
title = {Pristine or Highly Defective? Understanding the Role of Graphene Structure for Stable Lithium Metal Plating},
author = {Liu, Wei and Xia, Yuting and Wang, Wenwu and Wang, Yizhe and Jin, Jialun and Chen, Yungui and Paek, Eunsu and Mitlin, David},
abstractNote = {Abstract The role of graphene host structure/chemistry in plating–stripping in lithium metal anodes employed for lithium metal batteries is first examined in this study. Structural and chemical defects are bad, since highly defective graphene promotes unstable solid electrolyte interphase (SEI) growth. This consumes the fluoroethylene carbonate (FEC) additive in the carbonate electrolyte and is correlated with rapid decay in Coulombic efficiency (CE) and formation of filament‐like Li dendrites. A unique flow‐aided sonication exfoliation method is employed to synthesize “defect‐free” graphene (df‐G), allowing for a direct performance comparison with conventional reduced graphene oxide (r‐GO). At cycle 1, the r‐GO is better electrochemically wetted by Li than df‐G, indicating that initially it is more lithiophilic. With cycling, the nucleation overpotential with r‐GO becomes higher than with df‐G, indicating less facile plating reactions. The df‐G yields state‐of‐the‐art electrochemical performance, with the post cycled metal surface being relatively smooth and dendrite‐free. Conversely, r‐GO templates have CE rapidly degrade from the onset, with extensive dendrites after cycling. Severe SEI growth and associated FEC depletion with r‐GO are further confirmed by electrochemical impedance analysis and surface science methods. A new design rule is provided for Li metal templates: An ideal host must be noncatalytic toward SEI formation.},
doi = {10.1002/aenm.201802918},
journal = {Advanced Energy Materials},
number = 3,
volume = 9,
place = {United States},
year = {Tue Nov 27 00:00:00 EST 2018},
month = {Tue Nov 27 00:00:00 EST 2018}
}

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