Negating interfacial impedance in garnet-based solid-state Li metal batteries
Abstract
Garnet-type solid-state electrolytes have attracted extensive attention due to their high ionic conductivity, approaching 1 mS cm-1, excellent environmental stability, and wide electrochemical stability window, from lithium metal to ~6 V. However, to date, there has been little success in the development of high-performance solid-state batteries using these exceptional materials, the major challenge being the high solid–solid interfacial impedance between the garnet electrolyte and electrode materials. In this paper, we effectively address the large interfacial impedance between a lithium metal anode and the garnet electrolyte using ultrathin aluminium oxide (Al2O3) by atomic layer deposition. Li7La2.75Ca0.25Zr1.75Nb0.25O12 (LLCZN) is the garnet composition of choice in this work due to its reduced sintering temperature and increased lithium ion conductivity. A significant decrease of interfacial impedance, from 1,710 Ω cm2 to 1 Ω cm2, was observed at room temperature, effectively negating the lithium metal/garnet interfacial impedance. Experimental and computational results reveal that the oxide coating enables wetting of metallic lithium in contact with the garnet electrolyte surface and the lithiated-alumina interface allows effective lithium ion transport between the lithium metal anode and garnet electrolyte. Finally, we also demonstrate a working cell with a lithium metal anode, garnet electrolyte and a high-voltage cathode by applyingmore »
- Authors:
-
[1];
- Univ. of Maryland, College Park, MD (United States). Energy Research Center. Dept. of Materials Science and Engineering
- (Kelvin) [Univ. of Maryland, College Park, MD (United States). Energy Research Center. Dept. of Materials Science and Engineering
- Univ. of Maryland, College Park, MD (United States). Energy Research Center. Dept. of Materials Science and Engineering. Inst. for Systems Research
- Univ. of Calgary, AB (Canada). Dept. of Chemistry
- Publication Date:
- Research Org.:
- Univ. of Maryland, College Park, MD (United States)
- Sponsoring Org.:
- USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V); USDOE Advanced Research Projects Agency - Energy (ARPA-E); USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)
- OSTI Identifier:
- 1433807
- Grant/Contract Number:
- EE0006860; AR0000384; SC0001160; DMR150038
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Nature Materials
- Additional Journal Information:
- Journal Volume: 16; Journal Issue: 5; Journal ID: ISSN 1476-1122
- Publisher:
- Nature Publishing Group
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 25 ENERGY STORAGE; batteries
Citation Formats
Han, Xiaogang, Gong, Yunhui, Fu, Kun, He, Xingfeng, Hitz, Gregory T., Dai, Jiaqi, Pearse, Alex, Liu, Boyang, Wang, Howard, Rubloff, Gary, Mo, Yifei, Thangadurai, Venkataraman, Wachsman, Eric D., and Hu, Liangbing. Negating interfacial impedance in garnet-based solid-state Li metal batteries. United States: N. p., 2016.
Web. doi:10.1038/nmat4821.
Han, Xiaogang, Gong, Yunhui, Fu, Kun, He, Xingfeng, Hitz, Gregory T., Dai, Jiaqi, Pearse, Alex, Liu, Boyang, Wang, Howard, Rubloff, Gary, Mo, Yifei, Thangadurai, Venkataraman, Wachsman, Eric D., & Hu, Liangbing. Negating interfacial impedance in garnet-based solid-state Li metal batteries. United States. https://doi.org/10.1038/nmat4821
Han, Xiaogang, Gong, Yunhui, Fu, Kun, He, Xingfeng, Hitz, Gregory T., Dai, Jiaqi, Pearse, Alex, Liu, Boyang, Wang, Howard, Rubloff, Gary, Mo, Yifei, Thangadurai, Venkataraman, Wachsman, Eric D., and Hu, Liangbing. Mon .
"Negating interfacial impedance in garnet-based solid-state Li metal batteries". United States. https://doi.org/10.1038/nmat4821. https://www.osti.gov/servlets/purl/1433807.
@article{osti_1433807,
title = {Negating interfacial impedance in garnet-based solid-state Li metal batteries},
author = {Han, Xiaogang and Gong, Yunhui and Fu, Kun and He, Xingfeng and Hitz, Gregory T. and Dai, Jiaqi and Pearse, Alex and Liu, Boyang and Wang, Howard and Rubloff, Gary and Mo, Yifei and Thangadurai, Venkataraman and Wachsman, Eric D. and Hu, Liangbing},
abstractNote = {Garnet-type solid-state electrolytes have attracted extensive attention due to their high ionic conductivity, approaching 1 mS cm-1, excellent environmental stability, and wide electrochemical stability window, from lithium metal to ~6 V. However, to date, there has been little success in the development of high-performance solid-state batteries using these exceptional materials, the major challenge being the high solid–solid interfacial impedance between the garnet electrolyte and electrode materials. In this paper, we effectively address the large interfacial impedance between a lithium metal anode and the garnet electrolyte using ultrathin aluminium oxide (Al2O3) by atomic layer deposition. Li7La2.75Ca0.25Zr1.75Nb0.25O12 (LLCZN) is the garnet composition of choice in this work due to its reduced sintering temperature and increased lithium ion conductivity. A significant decrease of interfacial impedance, from 1,710 Ω cm2 to 1 Ω cm2, was observed at room temperature, effectively negating the lithium metal/garnet interfacial impedance. Experimental and computational results reveal that the oxide coating enables wetting of metallic lithium in contact with the garnet electrolyte surface and the lithiated-alumina interface allows effective lithium ion transport between the lithium metal anode and garnet electrolyte. Finally, we also demonstrate a working cell with a lithium metal anode, garnet electrolyte and a high-voltage cathode by applying the newly developed interface chemistry.},
doi = {10.1038/nmat4821},
journal = {Nature Materials},
number = 5,
volume = 16,
place = {United States},
year = {Mon Dec 19 00:00:00 EST 2016},
month = {Mon Dec 19 00:00:00 EST 2016}
}
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Ceramic Nanoparticle-Decorated Melt-Electrospun PVDF Nanofiber Membrane with Enhanced Performance as a Lithium-Ion Battery Separator
journal, September 2019
- Wu, Shuanglin; Ning, Jingxia; Jiang, Feng
- ACS Omega, Vol. 4, Issue 15
Solubility-mediated sustained release enabling nitrate additive in carbonate electrolytes for stable lithium metal anode
journal, September 2018
- Liu, Yayuan; Lin, Dingchang; Li, Yuzhang
- Nature Communications, Vol. 9, Issue 1
Advanced sulfide solid electrolyte by core-shell structural design
journal, October 2018
- Wu, Fan; Fitzhugh, William; Ye, Luhan
- Nature Communications, Vol. 9, Issue 1
A complex hydride lithium superionic conductor for high-energy-density all-solid-state lithium metal batteries
journal, March 2019
- Kim, Sangryun; Oguchi, Hiroyuki; Toyama, Naoki
- Nature Communications, Vol. 10, Issue 1
Tuning wettability of molten lithium via a chemical strategy for lithium metal anodes
journal, October 2019
- Wang, Shu-Hua; Yue, Junpei; Dong, Wei
- Nature Communications, Vol. 10, Issue 1
Investigation on the interface between Li10GeP2S12 electrolyte and carbon conductive agents in all-solid-state lithium battery
journal, May 2018
- Yoon, Kyungho; Kim, Jung-Joon; Seong, Won Mo
- Scientific Reports, Vol. 8, Issue 1
Towards high energy density lithium battery anodes: silicon and lithium
journal, January 2019
- Zhu, Bin; Wang, Xinyu; Yao, Pengcheng
- Chemical Science, Vol. 10, Issue 30
Lattice-geometry effects in garnet solid electrolytes: a lattice-gas Monte Carlo simulation study
journal, November 2017
- Morgan, Benjamin J.
- Royal Society Open Science, Vol. 4, Issue 11
Transforming from planar to three-dimensional lithium with flowable interphase for solid lithium metal batteries
journal, October 2017
- Liu, Yayuan; Lin, Dingchang; Jin, Yang
- Science Advances, Vol. 3, Issue 10
Pascalammetry with operando microbattery probes: Sensing high stress in solid-state batteries
journal, June 2018
- Larson, Jonathan M.; Gillette, Eleanor; Burson, Kristen
- Science Advances, Vol. 4, Issue 6
Interfaces Between Cathode and Electrolyte in Solid State Lithium Batteries: Challenges and Perspectives
journal, December 2018
- Nie, Kaihui; Hong, Yanshuai; Qiu, Jiliang
- Frontiers in Chemistry, Vol. 6
Graphene-Modified 3D Copper Foam Current Collector for Dendrite-Free Lithium Deposition
journal, November 2019
- Yu, Juan; Dang, Yangyang; Bai, Maohui
- Frontiers in Chemistry, Vol. 7
Lithiophilic Silver Coating on Lithium Metal Surface for Inhibiting Lithium Dendrites
journal, February 2020
- Zuo, Zefu; Zhuang, Libin; Xu, Jinzhuo
- Frontiers in Chemistry, Vol. 8
Arsenic Uptake, Toxicity, Detoxification, and Speciation in Plants: Physiological, Biochemical, and Molecular Aspects
journal, January 2018
- Abbas, Ghulam; Murtaza, Behzad; Bibi, Irshad
- International Journal of Environmental Research and Public Health, Vol. 15, 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