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Negating interfacial impedance in garnet-based solid-state Li metal batteries

Journal Article · · Nature Materials
DOI:https://doi.org/10.1038/nmat4821· OSTI ID:1433807
 [1];  [2];  [2];  [2];  [2];  [2];  [3];  [2];  [2];  [3];  [2];  [4];  [2];  [2]
  1. Univ. of Maryland, College Park, MD (United States). Energy Research Center. Dept. of Materials Science and Engineering; University of Maryland
  2. Univ. of Maryland, College Park, MD (United States). Energy Research Center. Dept. of Materials Science and Engineering
  3. Univ. of Maryland, College Park, MD (United States). Energy Research Center. Dept. of Materials Science and Engineering. Inst. for Systems Research
  4. Univ. of Calgary, AB (Canada). Dept. of Chemistry
Garnet-type solid-state electrolytes have attracted extensive attention due to their high ionic conductivity, approaching 1 mS cm-1, excellent environmental stability, and wide electrochemical stability window, from lithium metal to ~6 V. However, to date, there has been little success in the development of high-performance solid-state batteries using these exceptional materials, the major challenge being the high solid–solid interfacial impedance between the garnet electrolyte and electrode materials. In this paper, we effectively address the large interfacial impedance between a lithium metal anode and the garnet electrolyte using ultrathin aluminium oxide (Al2O3) by atomic layer deposition. Li7La2.75Ca0.25Zr1.75Nb0.25O12 (LLCZN) is the garnet composition of choice in this work due to its reduced sintering temperature and increased lithium ion conductivity. A significant decrease of interfacial impedance, from 1,710 Ω cm2 to 1 Ω cm2, was observed at room temperature, effectively negating the lithium metal/garnet interfacial impedance. Experimental and computational results reveal that the oxide coating enables wetting of metallic lithium in contact with the garnet electrolyte surface and the lithiated-alumina interface allows effective lithium ion transport between the lithium metal anode and garnet electrolyte. Finally, we also demonstrate a working cell with a lithium metal anode, garnet electrolyte and a high-voltage cathode by applying the newly developed interface chemistry.
Research Organization:
Univ. of Maryland, College Park, MD (United States)
Sponsoring Organization:
National Science Foundation (NSF) (United States); USDOE Advanced Research Projects Agency - Energy (ARPA-E); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Grant/Contract Number:
AR0000384; EE0006860; SC0001160
OSTI ID:
1433807
Alternate ID(s):
OSTI ID: 1388692
Journal Information:
Nature Materials, Journal Name: Nature Materials Journal Issue: 5 Vol. 16; ISSN 1476-1122
Publisher:
Nature Publishing GroupCopyright Statement
Country of Publication:
United States
Language:
English

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Building better all-solid-state batteries with Li-garnet solid electrolytes and metalloid anodes text January 2019
Lattice-Geometry Effects in Garnet Solid Electrolytes: A Lattice-Gas Monte Carlo Simulation Study preprint January 2017

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