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Comparative Analysis of Reactivity of Al and Ga Doped Garnet Solid State Electrolyte at the Interface with Li Metal

Journal Article · · ACS Materials Letters
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  1. Argonne National Laboratory (ANL), Argonne, IL (United States)
  2. Technische Univ. München, Garching (Germany). Heinz Maier-Leibnitz Zentrum (MLZ)
  3. Czech Academy of Sciences (CAS), Rez (Czech Republic)
  4. Univ. of California, Santa Barbara, CA (United States)
+ Show Author Affiliations
Lithium garnet (Li7La3Zr2O12, LLZO) based solid electrolytes are leading candidate materials for all-solid-state batteries with lithium metal anodes because of their high ionic conductivity, high mechanical toughness, and superior electrochemical stability. While doping LLZO with Al and Ga increases its ionic conductivity by stabilizing the cubic phase, the impact of dopants on its (electro)chemical stability at the interfaces with Li metal is critical. Here, our study of differences between Al- and Ga-doped LLZO when interfaced with lithium metal using X-ray photoelectron spectroscopy and density functional theory shows a higher propensity of Ga to move across LLZO interface with Li metal and form Ga-Li alloy. Additionally, neutron diffraction reveals loss of cubic phase resulting from the loss of dopant that explains electrochemical behavior differences between Ga- and Al-doped LLZO. Overall, our study reveals the key role of dopant chemistry in enabling stable solid electrolyte materials for all-solid-state batteries.
Research Organization:
Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Organization:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Vehicle Technologies Office (VTO)
Grant/Contract Number:
AC02-06CH11357
OSTI ID:
2997243
Journal Information:
ACS Materials Letters, Journal Name: ACS Materials Letters Journal Issue: 12 Vol. 6; ISSN 2639-4979
Publisher:
American Chemical Society (ACS)Copyright Statement
Country of Publication:
United States
Language:
English

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