Atomic Layer Deposition of the Solid Electrolyte Garnet Li ₇ La ₃ Zr ₂ O ₁₂

Journal Article · Thu Apr 13 04:00:00 EDT 2017 · Chemistry of Materials

DOI:https://doi.org/10.1021/acs.chemmater.7b00944· OSTI ID:1390428

Kazyak, Eric ^[1]; Chen, Kuan-Hung ^[1]; Wood, Kevin N. ^[1]; Davis, Andrew L. ^[1]; Thompson, Travis ^[1]; Bielinski, Ashley R. ^[1]; Sanchez, Adrian J. ^[1]; Wang, Xiang ^[2]; Wang, Chongmin ^[3]; Sakamoto, Jeff ^[1]; Dasgupta, Neil P. ^[1]

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1. Department of Mechanical Engineering, University of Michigan, Ann Arbor, Michigan 48109, United States
2. Department of Mechanical Engineering and Materials Science, University of Pittsburgh, Pittsburgh, Pennsylvania 15261, United States
3. Environmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory, Richland, Washington 99354, United States

Lithium solid electrolytes are a promising platform for achieving high energy density, long-lasting, and safe rechargeable batteries, which could have widespread societal impact. In particular, the ceramic oxide garnet Li7La3Zr2O12 (LLZO) has been shown to be a promising electrolyte due to its stability and high ionic conductivity. Two major challenges for commercialization are manufacturing of thin layers and creating stable, low-impedance, interfaces with both anode and cathode materials. Atomic Layer Deposition (ALD) has recently been shown as a potential method for depositing both solid electrolytes and interfacial layers to improve the stability and performance at electrode-electrolyte interfaces in battery systems. Herein we present the first reported ALD process for LLZO, demonstrating the ability to tune composition within the amorphous film and anneal to achieve the desired cubic garnet phase. Formation of the cubic phase was observed at temperatures as low as 555°C, significantly lower than is required for bulk processing. Additionally, challenges associated with achieving a dense garnet phase due to substrate reactivity, morphology changes and Li loss under the necessary high temperature annealing are quantified via in situ synchrotron diffraction.

• Research Organization: Pacific Northwest National Laboratory (PNNL), Richland, WA (US), Environmental Molecular Sciences Laboratory (EMSL)
• Sponsoring Organization: USDOE Advanced Research Projects Agency - Energy (ARPA-E)
• DOE Contract Number: AC05-76RL01830
• OSTI ID: 1390428
• Report Number(s): PNNL-SA-124464; 48885; KP1704020
• Journal Information: Chemistry of Materials, Journal Name: Chemistry of Materials Journal Issue: 8 Vol. 29; ISSN 0897-4756
• Publisher: American Chemical Society (ACS)
• Country of Publication: United States
• Language: English

Related Subjects

Atomic layer deposition
Environmental Molecular Sciences Laboratory
LLZO
garnet
solid electrolyte