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In Situ Plating of Porous Mg Network Layer to Reinforce Anode Dendrite Suppression in Li-Metal Batteries

  • Fulu Chu
    Fulu Chu
    School of Materials Science and Engineering, Xiangtan University, Xiangtan 411105, China
    State Key Laboratory of High Performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics, Chinese Academy of Sciences, 1295 Ding Xi Road, Shanghai 200050, China
    More by Fulu Chu
    • , 
  • Jiulin Hu
    Jiulin Hu
    State Key Laboratory of High Performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics, Chinese Academy of Sciences, 1295 Ding Xi Road, Shanghai 200050, China
    More by Jiulin Hu
    • , 
  • Jing Tian
    Jing Tian
    State Key Laboratory of High Performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics, Chinese Academy of Sciences, 1295 Ding Xi Road, Shanghai 200050, China
    More by Jing Tian
    • , 
  • Xuejun Zhou
    Xuejun Zhou
    State Key Laboratory of High Performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics, Chinese Academy of Sciences, 1295 Ding Xi Road, Shanghai 200050, China
    More by Xuejun Zhou
    • , 
  • Zheng Li*
    Zheng Li
    School of Materials Science and Engineering, Xiangtan University, Xiangtan 411105, China
    *E-mail: [email protected] (Z.L.).
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    • , and 
  • Chilin Li*
    Chilin Li
    State Key Laboratory of High Performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics, Chinese Academy of Sciences, 1295 Ding Xi Road, Shanghai 200050, China
    *E-mail: [email protected] (C.L.).
    More by Chilin Li
    Orcidhttp://orcid.org/0000-0002-5587-8617
Cite this: ACS Appl. Mater. Interfaces 2018, 10, 15, 12678–12689
Publication Date (Web):March 23, 2018
https://doi.org/10.1021/acsami.8b00989
Copyright © 2018 American Chemical Society
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Abstract

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Li dendrite suppression enables a highly reversible Li-metal battery. However the strategy to smooth Li surface, especially under long-term cycling and high current density, is still a big challenge. Here, we propose a facile additive strategy to reinforce Li dendrite inhibition in a range of ether and carbonate electrolytes. Dissoluble Mg(TFSI)2 is employed as a degradable electrolyte additive, leading to in situ plating of porous Mg network when contacting reductive Li atoms. Mg adatoms with extremely low diffusion energy barrier as lithiophilic sites enable a smooth or flaky morphology of Li surface even under a high current density of 2 mA/cm2 and high capacity of 6 mAh/cm2. Mg-salt additive significantly extends the cycling life of Li||Cu asymmetric cells up to 240 and 200 cycles for carbonate and ether electrolytes, respectively. Under a current density as high as 5 mA/cm2, the Li||Cu cell based on ether system can still survive up to 140 cycles with a small voltage hysteresis close to 60 mV. The hysteresis can be reduced to below 25 mV for lasting 200 cycles at 1 mA/cm2. This additive strategy provides a facile solution to in situ construction of conductive anode–electrolyte interface with low interface resistance for alleviating uneven Li nucleation.

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The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acsami.8b00989.

  • Voltage gap of Li||Li symmetric cells for 0 and 25 mM Mg(TFSI)2-contained DGM–LiTFSI and EC–DMC–LiPF6 systems; voltage profiles of Li||Cu asymmetric cells for 0 and 25 mM Mg(TFSI)2-contained EC–DMC–LiPF6 and DOL–DME–LiTFSI–LiNO3 systems; Coulombic efficiency of Li||Cu asymmetric cells in DOL–DME–LiTFSI–LiNO3 systems with 0 and 25 mM Mg(TFSI)2; voltage hysteresis of Li||Cu asymmetric cells for 0 and 25 mM Mg(TFSI)2-contained DOL–DME–LiTFSI–LiNO3 systems; impedance spectra of Li||Li symmetric cells for 0 and 25 mM Mg(TFSI)2-contained EC–DMC–LiPF6 systems; XPS spectra of cycled Li anode for Mg(TFSI)2-free and -contained LiTFSI–DGM systems; rate performance and Coulombic efficiency of Li/LiFePO4 cells based on Mg(TFSI)2-contained EC–DMC–LiPF6 electrolyte (PDF)

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This article is cited by 31 publications.

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