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

Liu, Wei; Xia, Yuting; Wang, Wenwu; Wang, Yizhe; Jin, Jialun; Chen, Yungui; Paek, Eunsu; Mitlin, David

doi:10.1002/aenm.201802918

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

Journal Article · 26 November 2018 · Advanced Energy Materials

DOI: https://doi.org/10.1002/aenm.201802918 · OSTI ID:1612832

^[1]; Xia, Yuting ^[2]; Wang, Wenwu ^[2]; Wang, Yizhe ^[2]; Jin, Jialun ^[2]; Chen, Yungui ^[3]; Paek, Eunsu ^[4];

^[5]

Sichuan Univ., Chengdu (China). Inst. of New-Energy and Low-Carbon Technology; DOE/OSTI
Sichuan Univ., Chengdu (China). Inst. of New-Energy and Low-Carbon Technology
Sichuan Univ., Chengdu (China). Inst. of New-Energy and Low-Carbon Technology; Sichuan Univ., Chengdu (China)
Clarkson Univ., Potsdam, NY (United States)
Sichuan Univ., Chengdu (China). Inst. of New-Energy and Low-Carbon Technology; Clarkson Univ., Potsdam, NY (United States)

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. Finally, a new design rule is provided for Li metal templates: An ideal host must be noncatalytic toward SEI formation.

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Research Organization:: Clarkson Univ., Potsdam, NY (United States)

Sponsoring Organization:: China Postdoctoral Science Foundation; National Natural Science Foundation of China (NSFC); USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division

Grant/Contract Number:: SC0018074

OSTI ID:: 1612832

Journal Information:: Advanced Energy Materials, Journal Name: Advanced Energy Materials Journal Issue: 3 Vol. 9; ISSN 1614-6832

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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A functional SrF ₂ coated separator enabling a robust and dendrite-free solid electrolyte interphase on a lithium metal anode Li, Xing; Liu, Yang; Pan, Yong Journal of Materials Chemistry A, Vol. 7, Issue 37 https://doi.org/10.1039/c9ta06908a	journal	January 2019
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