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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 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 metalmore » 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]
+ Show Author Affiliations
  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:
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.
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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. https://doi.org/10.1126/sciadv.1601659
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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. https://doi.org/10.1126/sciadv.1601659. https://www.osti.gov/servlets/purl/1425393.
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@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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https://doi.org/10.1126/sciadv.1601659
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    journal, July 2019

    High Uptake and Fast Transportation of LiPF 6 in a Porous Aromatic Framework for Solid‐State Li‐Ion Batteries
    journal, December 2019

    Transient Behavior of the Metal Interface in Lithium Metal-Garnet Batteries
    journal, October 2017

    • Fu, Kun Kelvin; Gong, Yunhui; Fu, Zhezhen
    • Angewandte Chemie International Edition, Vol. 56, Issue 47
    • DOI: 10.1002/anie.201708637

    High Uptake and Fast Transportation of LiPF 6 in a Porous Aromatic Framework for Solid‐State Li‐Ion Batteries
    journal, January 2020

    • Zou, Junyan; Trewin, Abbie; Ben, Teng
    • Angewandte Chemie International Edition, Vol. 59, Issue 2
    • DOI: 10.1002/anie.201913380

    Reducing the Interfacial Resistance in All‐Solid‐State Lithium Batteries Based on Oxide Ceramic Electrolytes
    journal, April 2019

    Synthesis and Properties of NaSICON‐type LATP and LAGP Solid Electrolytes
    journal, July 2019

    Design Principles of the Anode–Electrolyte Interface for All Solid‐State Lithium Metal Batteries
    journal, October 2019

    Using in operando diffraction to relate lattice strain with degradation mechanism in a NMC battery
    journal, October 2018

    • Jha, Shikhar Krishn; Charalambous, Harry; Okasinski, John S.
    • Journal of Materials Science, Vol. 54, Issue 3
    • DOI: 10.1007/s10853-018-3007-8

    Infiltrating lithium into carbon cloth decorated with zinc oxide arrays for dendrite-free lithium metal anode
    journal, November 2018

    Rechargeable solid-state Li-air batteries: a status report
    journal, April 2018

    Solid-State Electrolytes for Lithium-Ion Batteries: Fundamentals, Challenges and Perspectives
    journal, August 2019

    Diatomite derived hierarchical hybrid anode for high performance all-solid-state lithium metal batteries
    journal, June 2019

    Tuning wettability of molten lithium via a chemical strategy for lithium metal anodes
    journal, October 2019

    A low ride on processing temperature for fast lithium conduction in garnet solid-state battery films
    journal, May 2019

    Reviving lithium cobalt oxide-based lithium secondary batteries-toward a higher energy density
    journal, January 2018

    • Wang, Longlong; Chen, Bingbing; Ma, Jun
    • Chemical Society Reviews, Vol. 47, Issue 17
    • DOI: 10.1039/c8cs00322j

    Rationalizing the interphase stability of Li|doped-Li 7 La 3 Zr 2 O 12 via automated reaction screening and machine learning
    journal, January 2019

    • Liu, Bo; Yang, Jiong; Yang, Hongliang
    • Journal of Materials Chemistry A, Vol. 7, Issue 34
    • DOI: 10.1039/c9ta06748e

    Continuous plating/stripping behavior of solid-state lithium metal anode in a 3D ion-conductive framework
    journal, March 2018

    • Yang, Chunpeng; Zhang, Lei; Liu, Boyang
    • Proceedings of the National Academy of Sciences, Vol. 115, Issue 15
    • DOI: 10.1073/pnas.1719758115

    Stitching h-BN by atomic layer deposition of LiF as a stable interface for lithium metal anode
    journal, November 2017

    Upgrading traditional liquid electrolyte via in situ gelation for future lithium metal batteries
    journal, October 2018

    Review—Li Metal Anode in Working Lithium-Sulfur Batteries
    journal, June 2017

    • Cheng, Xin-Bing; Huang, Jia-Qi; Zhang, Qiang
    • Journal of The Electrochemical Society, Vol. 165, Issue 1
    • DOI: 10.1149/2.0111801jes

    Defect Detection in Solid-State Battery Electrolytes Using Lock-In Thermal Imaging
    journal, January 2018

    • Sulas, Dana B.; Johnston, Steve; Seitzman, Natalie
    • Journal of The Electrochemical Society, Vol. 165, Issue 13
    • DOI: 10.1149/2.0131814jes

    Communication—Demonstration and Electrochemistry of a Self-Forming Solid State Rechargeable LiI(HPN) 2 Based Li/I 2 Battery
    journal, January 2018

    • Abraham, Alyson; Huang, Jianping; Smith, Paul F.
    • Journal of The Electrochemical Society, Vol. 165, Issue 10
    • DOI: 10.1149/2.0371810jes

    Combinatorial Methods for Improving Lithium Metal Cycling Efficiency
    journal, January 2018

    • Genovese, Matthew; Louli, A. J.; Weber, Rochelle
    • Journal of The Electrochemical Society, Vol. 165, Issue 13
    • DOI: 10.1149/2.0401813jes

    Towards Mixed Ionic and Electronic Conducting Li-Stuffed Garnets
    journal, January 2018

    • Samson, Alfred Junio; Hofstetter, Kyle; Wachsman, Eric
    • Journal of The Electrochemical Society, Vol. 165, Issue 10
    • DOI: 10.1149/2.1001810jes

    Research Progress of the Solid State Lithium-Sulfur Batteries
    journal, October 2019

    Mixed Ionic and Electronic Conductor for Li-Metal Anode Protection
    journal, January 2018

    Borohydride-Scaffolded Li/Na/Mg Fast Ionic Conductors for Promising Solid-State Electrolytes
    journal, October 2018

    Interphases, Interfaces, and Surfaces of Active Materials in Rechargeable Batteries and Perovskite Solar Cells
    journal, January 2020

    A Material Perspective of Rechargeable Metallic Lithium Anodes
    journal, February 2018

    Perovskite Membranes with Vertically Aligned Microchannels for All-Solid-State Lithium Batteries
    journal, August 2018

    • Jiang, Zhouyang; Xie, Huiqi; Wang, Suqing
    • Advanced Energy Materials, Vol. 8, Issue 27
    • DOI: 10.1002/aenm.201801433

    Interfacial Incompatibility and Internal Stresses in All‐Solid‐State Lithium Ion Batteries
    journal, August 2019

    • He, Yanming; Lu, Chuanyang; Liu, Shan
    • Advanced Energy Materials, Vol. 9, Issue 36
    • DOI: 10.1002/aenm.201901810

    Diffusion Limitation of Lithium Metal and Li–Mg Alloy Anodes on LLZO Type Solid Electrolytes as a Function of Temperature and Pressure
    journal, October 2019

    • Krauskopf, Thorben; Mogwitz, Boris; Rosenbach, Carolin
    • Advanced Energy Materials, Vol. 9, Issue 44
    • DOI: 10.1002/aenm.201902568

    Solid‐State Lithium Batteries: Bipolar Design, Fabrication, and Electrochemistry
    journal, May 2019

    • Jung, Kyu‐Nam; Shin, Hyun‐Seop; Park, Min‐Sik
    • ChemElectroChem, Vol. 6, Issue 15
    • DOI: 10.1002/celc.201900736

    A review of solid electrolytes for safe lithium-sulfur batteries
    journal, November 2017

    Ultra-thin atom layer deposited alumina film enables the precise lifetime control of fully biodegradable electronic devices
    journal, January 2019

    • Huang, Shuyi; Xuan, Weipeng; Liu, Shuting
    • Nanoscale, Vol. 11, Issue 46
    • DOI: 10.1039/c9nr06566k

    A borate decorated anion-immobilized solid polymer electrolyte for dendrite-free, long-life Li metal batteries
    journal, January 2019

    • Ma, Cheng; Feng, Yiming; Xing, Fangzhou
    • Journal of Materials Chemistry A, Vol. 7, Issue 34
    • DOI: 10.1039/c9ta07551h

    An anion-immobilized composite electrolyte for dendrite-free lithium metal anodes
    journal, October 2017

    • Zhao, Chen-Zi; Zhang, Xue-Qiang; Cheng, Xin-Bing
    • Proceedings of the National Academy of Sciences, Vol. 114, Issue 42
    • DOI: 10.1073/pnas.1708489114

    Building Better Batteries in the Solid State: A Review
    journal, November 2019

    • Mauger, Alain; Julien, Christian M.; Paolella, Andrea
    • Materials, Vol. 12, Issue 23, p. 3892
    • DOI: 10.3390/ma12233892

    Transient Behavior of the Metal Interface in Lithium Metal-Garnet Batteries
    journal, October 2017

    A Perovskite Electrolyte That Is Stable in Moist Air for Lithium-Ion Batteries
    journal, June 2018

    • Li, Yutao; Xu, Henghui; Chien, Po-Hsiu
    • Angewandte Chemie International Edition, Vol. 57, Issue 28
    • DOI: 10.1002/anie.201804114

    Graphitic Carbon Nitride (g‐C 3 N 4 ): An Interface Enabler for Solid‐State Lithium Metal Batteries
    journal, January 2020

    • Huang, Ying; Chen, Bo; Duan, Jian
    • Angewandte Chemie International Edition, Vol. 59, Issue 9
    • DOI: 10.1002/anie.201914417

    In situ X-ray photoelectron spectroscopy investigation of the solid electrolyte interphase in a Li/Li6.4Ga0.2La3Zr2O12/LiFePO4 all-solid-state battery
    journal, June 2019

    • Liu, Zhen; Li, Guozhu; Borodin, Andriy
    • Journal of Solid State Electrochemistry, Vol. 23, Issue 7
    • DOI: 10.1007/s10008-019-04296-4

    Recent Progress in All-Solid-State Lithium−Sulfur Batteries Using High Li-Ion Conductive Solid Electrolytes
    journal, February 2019

    High Li + transference gel interface between solid-oxide electrolyte and cathode for quasi-solid lithium-ion batteries
    journal, January 2019

    • Subramani, Ramesh; Tseng, Yu-Hsien; Lee, Yuh-Lang
    • Journal of Materials Chemistry A, Vol. 7, Issue 19
    • DOI: 10.1039/c9ta02515d

    Communication—Li/Li 7 La 3 Zr 2 O 12 Interfacial Modification by Constructing a Layer of Cu-Li Alloy
    journal, January 2019

    • Xiang, Xing; Cao, Shiyu; Chen, Fei
    • Journal of The Electrochemical Society, Vol. 166, Issue 13
    • DOI: 10.1149/2.0651913jes

    Graphitic Carbon Nitride (g‐C 3 N 4 ): An Interface Enabler for Solid‐State Lithium Metal Batteries
    journal, January 2020

    Engineering stable interfaces for three-dimensional lithium metal anodes
    journal, July 2018

    Review—Practical Challenges Hindering the Development of Solid State Li Ion Batteries
    journal, January 2017

    • Kerman, Kian; Luntz, Alan; Viswanathan, Venkatasubramanian
    • Journal of The Electrochemical Society, Vol. 164, Issue 7
    • DOI: 10.1149/2.1571707jes

    A Perovskite Electrolyte That Is Stable in Moist Air for Lithium‐Ion Batteries
    journal, June 2018

    A 3D Lithium/Carbon Fiber Anode with Sustained Electrolyte Contact for Solid‐State Batteries
    journal, December 2019

    • Zhang, Ying; Shi, Yang; Hu, Xin‐Cheng
    • Advanced Energy Materials, Vol. 10, Issue 3
    • DOI: 10.1002/aenm.201903325

    Sol Gel vs Solid State Synthesis of the Fast Lithium-Ion Conducting Solid State Electrolyte Li 7 La 3 Zr 2 O 12 Substituted with Iron
    journal, January 2019

    • Paulus, Anja; Kammler, Simon; Heuer, Sabrina
    • Journal of The Electrochemical Society, Vol. 166, Issue 3
    • DOI: 10.1149/2.0641903jes

    Diatomite derived hierarchical hybrid anode for high performance all-solid-state lithium metal batteries
    journal, June 2019

    Tuning wettability of molten lithium via a chemical strategy for lithium metal anodes
    journal, October 2019

    Engineering stable interfaces for three-dimensional lithium metal anodes
    journal, July 2018

    Making Sense of Complex Carbon and Metal/Carbon Systems by Secondary Electron Hyperspectral Imaging
    text, January 2019

    • Abrams, Kerry J.; Dapor, Maurizio; Stehling, Nicola
    • Weinheim : Wiley-VCH
    • DOI: 10.34657/9127
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