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Title: Reducing Interfacial Resistance between Garnet-Structured Solid-State Electrolyte and Li-Metal Anode by a Germanium Layer

Authors:
 [1];  [2];  [3];  [3];  [3];  [3];  [2];  [3];  [3];  [2];  [2];  [2]
  1. Department of Materials Science and Engineering, University of Maryland, College Park MD 20742 USA, Department of Mechanical Engineering, University of Maryland, College Park MD 20742 USA
  2. Department of Materials Science and Engineering, University of Maryland, College Park MD 20742 USA, University of Maryland Energy Research Center, University of Maryland, College Park MD 20742 USA
  3. Department of Materials Science and Engineering, University of Maryland, College Park MD 20742 USA
Publication Date:
Sponsoring Org.:
USDOE
OSTI Identifier:
1401062
Grant/Contract Number:
DEEE0006860; DESC0001160
Resource Type:
Journal Article: Publisher's Accepted Manuscript
Journal Name:
Advanced Materials
Additional Journal Information:
Journal Volume: 29; Journal Issue: 22; Related Information: CHORUS Timestamp: 2017-10-20 16:22:45; Journal ID: ISSN 0935-9648
Publisher:
Wiley Blackwell (John Wiley & Sons)
Country of Publication:
Germany
Language:
English

Citation Formats

Luo, Wei, Gong, Yunhui, Zhu, Yizhou, Li, Yiju, Yao, Yonggang, Zhang, Ying, Fu, Kun Kelvin, Pastel, Glenn, Lin, Chuan-Fu, Mo, Yifei, Wachsman, Eric D., and Hu, Liangbing. Reducing Interfacial Resistance between Garnet-Structured Solid-State Electrolyte and Li-Metal Anode by a Germanium Layer. Germany: N. p., 2017. Web. doi:10.1002/adma.201606042.
Luo, Wei, Gong, Yunhui, Zhu, Yizhou, Li, Yiju, Yao, Yonggang, Zhang, Ying, Fu, Kun Kelvin, Pastel, Glenn, Lin, Chuan-Fu, Mo, Yifei, Wachsman, Eric D., & Hu, Liangbing. Reducing Interfacial Resistance between Garnet-Structured Solid-State Electrolyte and Li-Metal Anode by a Germanium Layer. Germany. doi:10.1002/adma.201606042.
Luo, Wei, Gong, Yunhui, Zhu, Yizhou, Li, Yiju, Yao, Yonggang, Zhang, Ying, Fu, Kun Kelvin, Pastel, Glenn, Lin, Chuan-Fu, Mo, Yifei, Wachsman, Eric D., and Hu, Liangbing. Tue . "Reducing Interfacial Resistance between Garnet-Structured Solid-State Electrolyte and Li-Metal Anode by a Germanium Layer". Germany. doi:10.1002/adma.201606042.
@article{osti_1401062,
title = {Reducing Interfacial Resistance between Garnet-Structured Solid-State Electrolyte and Li-Metal Anode by a Germanium Layer},
author = {Luo, Wei and Gong, Yunhui and Zhu, Yizhou and Li, Yiju and Yao, Yonggang and Zhang, Ying and Fu, Kun Kelvin and Pastel, Glenn and Lin, Chuan-Fu and Mo, Yifei and Wachsman, Eric D. and Hu, Liangbing},
abstractNote = {},
doi = {10.1002/adma.201606042},
journal = {Advanced Materials},
number = 22,
volume = 29,
place = {Germany},
year = {Tue Apr 18 00:00:00 EDT 2017},
month = {Tue Apr 18 00:00:00 EDT 2017}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record at 10.1002/adma.201606042

Citation Metrics:
Cited by: 17works
Citation information provided by
Web of Science

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  • Solid-state batteries are a promising option toward high energy and power densities due to the use of lithium (Li) metal as an anode. Among all solid electrolyte materials ranging from sulfides to oxides and oxynitrides, cubic garnet–type Li 7La 3Zr 2O 12 (LLZO) ceramic electrolytes are superior candidates because of their high ionic conductivity (10 -3 to 10 -4 S/cm) and good stability against Li metal. However, garnet solid electrolytes generally have poor contact with Li metal, which causes high resistance and uneven current distribution at the interface. To address this challenge, we demonstrate a strategy to engineer the garnetmore » solid electrolyte and the Li metal interface by forming an intermediary Li-metal alloy, which changes the wettability of the garnet surface (lithiophobic to lithiophilic) and reduces the interface resistance by more than an order of magnitude: 950 ohm·cm2 for the pristine garnet/Li and 75 ohm·cm 2 for the surface-engineered garnet/Li. Li 7La 2.75Ca 0.25Zr 1.75Nb 0.25O 12 (LLCZN) was selected as the solid-state electrolyte (SSE) in this work because of its low sintering temperature, stabilized cubic garnet phase, and high ionic conductivity. This low area-specific resistance enables a solid-state garnet SSE/Li metal configuration and promotes the development of a hybrid electrolyte system. The hybrid system uses the improved solid-state garnet SSE Li metal anode and a thin liquid electrolyte cathode interfacial layer. This work provides new ways to address the garnet SSE wetting issue against Li and get more stable cell performances based on the hybrid electrolyte system for Li-ion, Li-sulfur, and Li-oxygen batteries toward the next generation of Li metal batteries.« less
  • 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.more » 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.« less