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Title: Toward garnet electrolyte–based Li metal batteries: An ultrathin, highly effective, artificial solid-state electrolyte/metallic Li interface

Abstract

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 garnet 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 hybridmore » 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

Authors:
 [1];  [2];  [2];  [2];  [2]; ORCiD logo [2];  [2];  [2];  [2];  [2]; ORCiD logo [2];  [2];  [2]
  1. (Kelvin) [Univ. of Maryland, College Park, MD (United States)
  2. Univ. of Maryland, College Park, MD (United States)
Publication Date:
Research Org.:
Univ. of Maryland, College Park, MD (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE)
OSTI Identifier:
1425393
Grant/Contract Number:
EE0006860
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Science Advances
Additional Journal Information:
Journal Volume: 3; Journal Issue: 4; Journal ID: ISSN 2375-2548
Publisher:
AAAS
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE

Citation Formats

Fu, Kun, Gong, Yunhui, Liu, Boyang, Xu, Shaomao, Yao, Yonggang, Luo, Wei, Wang, Chengwei, Lacey, Steven D., Dai, Jiaqi, Chen, Yanan, Mo, Yifei, Wachsman, Eric, and Hu, Liangbing. Toward garnet electrolyte–based Li metal batteries: An ultrathin, highly effective, artificial solid-state electrolyte/metallic Li interface. United States: N. p., 2017. Web. doi:10.1126/sciadv.1601659.
Fu, Kun, Gong, Yunhui, Liu, Boyang, Xu, Shaomao, Yao, Yonggang, Luo, Wei, Wang, Chengwei, Lacey, Steven D., Dai, Jiaqi, Chen, Yanan, Mo, Yifei, Wachsman, Eric, & Hu, Liangbing. Toward garnet electrolyte–based Li metal batteries: An ultrathin, highly effective, artificial solid-state electrolyte/metallic Li interface. United States. doi:10.1126/sciadv.1601659.
Fu, Kun, Gong, Yunhui, Liu, Boyang, Xu, Shaomao, Yao, Yonggang, Luo, Wei, Wang, Chengwei, Lacey, Steven D., Dai, Jiaqi, Chen, Yanan, Mo, Yifei, Wachsman, Eric, and Hu, Liangbing. Fri . "Toward garnet electrolyte–based Li metal batteries: An ultrathin, highly effective, artificial solid-state electrolyte/metallic Li interface". United States. doi:10.1126/sciadv.1601659. https://www.osti.gov/servlets/purl/1425393.
@article{osti_1425393,
title = {Toward garnet electrolyte–based Li metal batteries: An ultrathin, highly effective, artificial solid-state electrolyte/metallic Li interface},
author = {Fu, Kun and Gong, Yunhui and Liu, Boyang and Xu, Shaomao and Yao, Yonggang and Luo, Wei and Wang, Chengwei and Lacey, Steven D. and Dai, Jiaqi and Chen, Yanan and Mo, Yifei and Wachsman, Eric and Hu, Liangbing},
abstractNote = {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 Li7La3Zr2O12 (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 garnet 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·cm2 for the surface-engineered garnet/Li. Li7La2.75Ca0.25Zr1.75Nb0.25O12 (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.},
doi = {10.1126/sciadv.1601659},
journal = {Science Advances},
number = 4,
volume = 3,
place = {United States},
year = {Fri Apr 07 00:00:00 EDT 2017},
month = {Fri Apr 07 00:00:00 EDT 2017}
}

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