Hybrid Polymer/Garnet Electrolyte with a Small Interfacial Resistance for Lithium-Ion Batteries
Abstract
Li7La3Zr2O12-based Li-rich garnets react with water and carbon dioxide in air to form a Li-ion insulating Li2CO3 layer on the surface of the garnet particles, which results in a large interfacial resistance for Li-ion transfer. In this work, we introduce LiF to garnet Li6.5La3Zr1.5Ta0.5O12 (LLZT) to increase the stability of the garnet electrolyte against moist air; the garnet LLZT-2 wt % LiF (LLZT-2LiF) has less Li2CO3 on the surface and shows a small interfacial resistance with Li metal, a solid polymer electrolyte, and organic-liquid electrolytes. Lastly, an all-solid-state Li/polymer/LLZT-2LiF/LiFePO4 battery has a high Coulombic efficiency and long cycle life; a Li-S cell with the LLZT-2LiF electrolyte as a separator, which blocks the polysulfide transport towards the Li-metal, also has high Coulombic efficiency and kept 93 % of its capacity after 100 cycles.
- Authors:
-
- Univ. of Texas, Austin, TX (United States)
- Shanghai Jiao Tong University, Shanghai (China)
- Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
- Publication Date:
- Research Org.:
- Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division; USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V)
- OSTI Identifier:
- 1505978
- Report Number(s):
- LA-UR-16-27139
Journal ID: ISSN 1433-7851
- Grant/Contract Number:
- 89233218CNA000001; SC0005397
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Angewandte Chemie (International Edition)
- Additional Journal Information:
- Journal Name: Angewandte Chemie (International Edition); Journal Volume: 56; Journal Issue: 3; Journal ID: ISSN 1433-7851
- Publisher:
- Wiley
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; 25 ENERGY STORAGE; all-solid-state battery; interfacial resistance; Li-rich garnet; Li-S battery; lithium fluoride
Citation Formats
Li, Yutao, Xu, Biyi, Xu, Henghui, Duan, Huanan, Lü, Xujie, Xin, Sen, Zhou, Weidong, Xue, Leigang, Fu, Gengtao, Manthiram, Arumugam, and Goodenough, John B. Hybrid Polymer/Garnet Electrolyte with a Small Interfacial Resistance for Lithium-Ion Batteries. United States: N. p., 2016.
Web. doi:10.1002/anie.201608924.
Li, Yutao, Xu, Biyi, Xu, Henghui, Duan, Huanan, Lü, Xujie, Xin, Sen, Zhou, Weidong, Xue, Leigang, Fu, Gengtao, Manthiram, Arumugam, & Goodenough, John B. Hybrid Polymer/Garnet Electrolyte with a Small Interfacial Resistance for Lithium-Ion Batteries. United States. https://doi.org/10.1002/anie.201608924
Li, Yutao, Xu, Biyi, Xu, Henghui, Duan, Huanan, Lü, Xujie, Xin, Sen, Zhou, Weidong, Xue, Leigang, Fu, Gengtao, Manthiram, Arumugam, and Goodenough, John B. Fri .
"Hybrid Polymer/Garnet Electrolyte with a Small Interfacial Resistance for Lithium-Ion Batteries". United States. https://doi.org/10.1002/anie.201608924. https://www.osti.gov/servlets/purl/1505978.
@article{osti_1505978,
title = {Hybrid Polymer/Garnet Electrolyte with a Small Interfacial Resistance for Lithium-Ion Batteries},
author = {Li, Yutao and Xu, Biyi and Xu, Henghui and Duan, Huanan and Lü, Xujie and Xin, Sen and Zhou, Weidong and Xue, Leigang and Fu, Gengtao and Manthiram, Arumugam and Goodenough, John B.},
abstractNote = {Li7La3Zr2O12-based Li-rich garnets react with water and carbon dioxide in air to form a Li-ion insulating Li2CO3 layer on the surface of the garnet particles, which results in a large interfacial resistance for Li-ion transfer. In this work, we introduce LiF to garnet Li6.5La3Zr1.5Ta0.5O12 (LLZT) to increase the stability of the garnet electrolyte against moist air; the garnet LLZT-2 wt % LiF (LLZT-2LiF) has less Li2CO3 on the surface and shows a small interfacial resistance with Li metal, a solid polymer electrolyte, and organic-liquid electrolytes. Lastly, an all-solid-state Li/polymer/LLZT-2LiF/LiFePO4 battery has a high Coulombic efficiency and long cycle life; a Li-S cell with the LLZT-2LiF electrolyte as a separator, which blocks the polysulfide transport towards the Li-metal, also has high Coulombic efficiency and kept 93 % of its capacity after 100 cycles.},
doi = {10.1002/anie.201608924},
journal = {Angewandte Chemie (International Edition)},
number = 3,
volume = 56,
place = {United States},
year = {Fri Dec 09 00:00:00 EST 2016},
month = {Fri Dec 09 00:00:00 EST 2016}
}
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Figures / Tables:
Figure 1: (a) XRD patterns of LLZT with different amounts of LiF, (b) The impedance plots of LLZT and LLZT-2LiF with ion–blocking Au electrodes, (c) C 1s spectrum of LLZT and LLZT–2LiF, (d) The impedance plots of LLZT and LLZT–2LiF with Li electrodes, the pellets thickness and surface area aremore »
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- Mauger, Alain; Julien, Christian M.; Paolella, Andrea
- Materials, Vol. 12, Issue 23, p. 3892
Dual Substitution and Spark Plasma Sintering to Improve Ionic Conductivity of Garnet Li7La3Zr2O12
journal, May 2019
- Dong, Zhencai; Xu, Chao; Wu, Yongmin
- Nanomaterials, Vol. 9, Issue 5
Development of the PEO Based Solid Polymer Electrolytes for All-Solid State Lithium Ion Batteries
journal, November 2018
- Jiang, Yu; Yan, Xuemin; Ma, Zhaofei
- Polymers, Vol. 10, Issue 11
Promises, Challenges, and Recent Progress of Inorganic Solid-State Electrolytes for All-Solid-State Lithium Batteries
journal, February 2018
- Gao, Zhonghui; Sun, Huabin; Fu, Lin
- Advanced Materials, Vol. 30, Issue 17
Advances in Interfaces between Li Metal Anode and Electrolyte
journal, December 2017
- Zhang, Xue-Qiang; Cheng, Xin-Bing; Zhang, Qiang
- Advanced Materials Interfaces, Vol. 5, Issue 2
Hybrid Lithium-Sulfur Batteries with an Advanced Gel Cathode and Stabilized Lithium-Metal Anode
journal, May 2018
- Xu, Henghui; Wang, Shaofei; Manthiram, Arumugam
- Advanced Energy Materials, Vol. 8, Issue 23
Transient Behavior of the Metal Interface in Lithium Metal-Garnet Batteries
journal, October 2017
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- Angewandte Chemie, Vol. 129, Issue 47
Tough Gel Electrolyte Using Double Polymer Network Design for the Safe, Stable Cycling of Lithium Metal Anode
journal, January 2018
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- Angewandte Chemie, Vol. 130, Issue 5
A 3D Nanostructured Hydrogel-Framework-Derived High-Performance Composite Polymer Lithium-Ion Electrolyte
journal, January 2018
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- Angewandte Chemie, Vol. 130, Issue 8
Hybrid Solid Polymer Electrolytes with Two‐Dimensional Inorganic Nanofillers
journal, June 2018
- Chua, Stephanie; Fang, Ruopian; Sun, Zhenhua
- Chemistry – A European Journal, Vol. 24, Issue 69
High-performance all-solid-state batteries enabled by salt bonding to perovskite in poly(ethylene oxide)
journal, August 2019
- Xu, Henghui; Chien, Po-Hsiu; Shi, Jianjian
- Proceedings of the National Academy of Sciences, Vol. 116, Issue 38
Research Progress of the Solid State Lithium-Sulfur Batteries
journal, October 2019
- Wang, HangChao; Cao, Xin; Liu, Wen
- Frontiers in Energy Research, Vol. 7
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
Microstrain and electrochemical performance of garnet solid electrolyte integrated in a hybrid battery cell
journal, January 2019
- Botros, Miriam; Scherer, Torsten; Popescu, Radian
- RSC Advances, Vol. 9, Issue 53
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, Vol. 130, Issue 28
Microstrain and electrochemical performance of garnet solid electrolyte integrated in a hybrid battery cell
text, January 2019
- Botros, M.; Scherer, T.; Popescu, R.
- Karlsruhe
A 3D Nanostructured Hydrogel-Framework-Derived High-Performance Composite Polymer Lithium-Ion Electrolyte
journal, January 2018
- Bae, Jiwoong; Li, Yutao; Zhang, Jun
- Angewandte Chemie International Edition, Vol. 57, Issue 8
Controllable two-dimensional movement and redistribution of lithium ions in metal oxides
journal, June 2019
- Tang, Xiufeng; Chen, Guoxin; Mo, Zhaopeng
- Nature Communications, Vol. 10, Issue 1
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
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