Nature Materials, volume 16, issue 5, pages 572-579

Negating interfacial impedance in garnet-based solid-state Li metal batteries

Xiaogang Han 1
Yunhui Gong 1
Kun Fu 1
Xingfeng He 1
Gregory T. Hitz 1
Jiaqi Dai 1
Alex Pearse 1, 2
Boyang Liu 1
Howard Wang 1
Gary Rubloff 1, 2
Yifei Mo 1
Venkataraman Thangadurai 3
Eric D. Wachsman 1
Liangbing Hu 1
Publication typeJournal Article
Publication date2016-12-19
Journal: Nature Materials
Quartile SCImago
Q1
Quartile WOS
Q1
Impact factor41.2
ISSN14761122, 14764660
General Chemistry
Condensed Matter Physics
General Materials Science
Mechanical Engineering
Mechanics of Materials
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 work, 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. 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. Garnet-type electrolytes are attractive for lithium metal batteries due to their high ionic conductivity. A strategy to decrease interfacial impedance between a lithium metal anode and garnet electrolyte is found promising for all-solid-state batteries.

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Han X. et al. Negating interfacial impedance in garnet-based solid-state Li metal batteries // Nature Materials. 2016. Vol. 16. No. 5. pp. 572-579.
GOST all authors (up to 50) Copy
Han X., Gong Y., Fu K., He X., Hitz G. T., Dai J., Pearse A., Liu B., Wang H., Rubloff G., Mo Y., Thangadurai V., Wachsman E. D., Hu L. Negating interfacial impedance in garnet-based solid-state Li metal batteries // Nature Materials. 2016. Vol. 16. No. 5. pp. 572-579.
RIS |
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RIS Copy
TY - JOUR
DO - 10.1038/nmat4821
UR - https://doi.org/10.1038/nmat4821
TI - Negating interfacial impedance in garnet-based solid-state Li metal batteries
T2 - Nature Materials
AU - Han, Xiaogang
AU - Gong, Yunhui
AU - Fu, Kun
AU - He, Xingfeng
AU - Hitz, Gregory T.
AU - Dai, Jiaqi
AU - Pearse, Alex
AU - Liu, Boyang
AU - Wang, Howard
AU - Rubloff, Gary
AU - Mo, Yifei
AU - Thangadurai, Venkataraman
AU - Wachsman, Eric D.
AU - Hu, Liangbing
PY - 2016
DA - 2016/12/19 00:00:00
PB - Springer Nature
SP - 572-579
IS - 5
VL - 16
SN - 1476-1122
SN - 1476-4660
ER -
BibTex |
Cite this
BibTex Copy
@article{2016_Han,
author = {Xiaogang Han and Yunhui Gong and Kun Fu and Xingfeng He and Gregory T. Hitz and Jiaqi Dai and Alex Pearse and Boyang Liu and Howard Wang and Gary Rubloff and Yifei Mo and Venkataraman Thangadurai and Eric D. Wachsman and Liangbing Hu},
title = {Negating interfacial impedance in garnet-based solid-state Li metal batteries},
journal = {Nature Materials},
year = {2016},
volume = {16},
publisher = {Springer Nature},
month = {dec},
url = {https://doi.org/10.1038/nmat4821},
number = {5},
pages = {572--579},
doi = {10.1038/nmat4821}
}
MLA
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MLA Copy
Han, Xiaogang, et al. “Negating interfacial impedance in garnet-based solid-state Li metal batteries.” Nature Materials, vol. 16, no. 5, Dec. 2016, pp. 572-579. https://doi.org/10.1038/nmat4821.
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