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A Highly Efficient All-Solid-State Lithium/Electrolyte Interface Induced by an Energetic Reaction

Journal Article · · Angewandte Chemie (International Edition)
 [1];  [1];  [2];  [1];  [1];  [2];  [1]
  1. Yale Univ., New Haven, CT (United States)
  2. Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)
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Garnet-phase solid-state electrolytes, with high ionic conductivity and wide electrochemical windows, promise safe and energy-dense Li metal batteries. However, integrating them with Li metal faces crucial challenges including large resistance and dendrite formation at the interface, and therefore current Li/garnet electrodes, albeit with delicate interfacial designs, cannot rival liquid-electrolyte Li metal electrodes in performance. In this work, we make use of the energetic chemical reaction between Zn(NO3)2 and Li to create a solid-state interface between Li metal and Li6.4La3Zr1.4Ta0.6O12 (LLZTO) electrolyte. This interlayer, composed of Zn, ZnLix alloy, Li3N, Li2O and other species, possesses strong affinities with both Li metal and LLZTO and affords highly efficient conductive pathways for Li+ transport through the interface. The unique structure and properties of the interlayer lead to Li metal anodes with longer cycle life, higher efficiency and better safety compared to the current best Li metal electrodes operating in liquid electrolytes while retaining comparable capacity, rate, and overpotential. Our all-solid-state Li||Li cells can operate at very demanding current-capacity conditions of 4 mA/cm2-8 mAh/cm2. Thousands of hours of continuous cycling are achieved at Coulombic efficiency > 99.5% without dendrite formation or side reactions with the electrolyte.
Research Organization:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Grant/Contract Number:
SC0012704
OSTI ID:
1631927
Alternate ID(s):
OSTI ID: 22947312
Report Number(s):
BNL--215969-2020-JAAM
Journal Information:
Angewandte Chemie (International Edition), Journal Name: Angewandte Chemie (International Edition) Journal Issue: 33 Vol. 59; ISSN 1433-7851
Publisher:
WileyCopyright Statement
Country of Publication:
United States
Language:
English

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Related Subjects

25 ENERGY STORAGE
Li metal anodes
electrode/electrolyte interface
garnet electrolytes
reaction-induced interlayers
solid-state batteries