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Manipulating Electric Double Layer Adsorption for Stable Solid-Electrolyte Interphase in 2.3 Ah Zn-Pouch Cells.

Yu Wang1,2, Bochun Liang1, Jiaxiong Zhu1

  • 1Department of Materials Science and Engineering, City University of Hong Kong, Kowloon, 999077, Hong Kong SAR, China.

Angewandte Chemie (International Ed. in English)
|March 31, 2023
PubMed
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A new understanding of solid-electrolyte interphase (SEI) formation in zinc metal batteries reveals electric double-layer adsorption, not bulk solvation, is key. Ether additives like 12-crown-4 create a robust SEI, enabling high-performance zinc batteries.

Area of Science:

  • Electrochemistry
  • Materials Science
  • Energy Storage

Background:

  • Reliable solid-electrolyte interphase (SEI) construction is crucial for reversible zinc metal (Zn 0 ) electrodes.
  • Conventional understanding focused on bulk solvation mechanisms for SEI formation.

Purpose of the Study:

  • To investigate the role of electric double-layer (EDL) adsorption in SEI formation.
  • To manipulate EDL adsorption and Zn 2+ solvation using ether additives.
  • To develop high-performance zinc metal batteries.

Main Methods:

  • Utilized ether additives (15-crown-5, 12-crown-4, triglyme) to modify EDL adsorption and Zn 2+ solvation.
  • Characterized the SEI structure formed with 12-crown-4, identifying inorganic and organic components.
Keywords:
Bulk SolvationCrown EtherElectric Double LayerPouch CellZn Anode

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  • Fabricated and tested Zn||Zn and Zn||Zn 0.25 V 2 O 5 ⋅nH 2 O pouch cells.

    • Main Results:

    • Identified EDL adsorption as the dominant mechanism for SEI structure, challenging the bulk solvation theory.
    • 12-crown-4 additive resulted in a stable, layered SEI (inorganic ZnF x /ZnS x inner layer, organic C-O-C outer layer).
    • Achieved high cumulative capacity (4250 mAh·cm -2 ) in a 100 cm 2 Zn||Zn cell at 10 mAh·cm -2 areal capacity.
    • Demonstrated a 2.3 Ah Zn||Zn 0.25 V 2 O 5 ⋅nH 2 O cell with 104 Wh·L cell -1 energy density, operating >70 days under demanding conditions.

    Conclusions:

    • EDL adsorption control via ether additives is a viable strategy for constructing robust SEIs in zinc metal batteries.
    • The developed SEI structure enhances electrode stability and enables high-energy-density, long-life aqueous zinc batteries.
    • This work paves the way for practical applications of high-performance zinc-based energy storage devices.