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Surface Chemistry Mechanism of Ultra-Low Interfacial Resistance in the Solid-State Electrolyte Li7La3Zr2O12
Abstract
The impact of surface chemistry on the interfacial resistance between the Li 7 La 3 Zr 2 O 12 (LLZO) solid-state electrolyte and a metallic Li electrode is revealed. Control of surface chemistry allows the interfacial resistance to be reduced to 2 Ω cm 2, lower than that of liquid electrolytes, without the need for interlayer coatings. A mechanistic understanding of the origins of ultra-low resistance is provided by quantitatively evaluating the linkages between interfacial chemistry, Li wettability, and electrochemical phenomena. A combination of Li contact angle measurements, X-ray photoelectron spectroscopy (XPS), first-principles calculations, and impedance spectroscopy demonstrates that the presence of common LLZO surface contaminants, Li 2 CO 3 and LiOH, result in poor wettability by Li and high interfacial resistance. On the basis of this mechanism, a simple procedure for removing these surface layers is demonstrated, which results in a dramatic increase in Li wetting and the elimination of nearly all interfacial resistance. The low interfacial resistance is maintained over one-hundred cycles and suggests a straightforward pathway to achieving high energy and power density solid-state batteries.
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Cites
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Cited by
Local electronic structure variation resulting in Li ‘filament’ formation within solid electrolytes
Liu, X., Garcia-Mendez, R., Lupini, A. R., Cheng, Y., Hood, Z. D., Han, F., Sharafi, A., Idrobo, J. C., Dudney, N. J., Wang, C., et al. (2021) · Nature Materials · doi:10.1038/s41563-021-01019-x · Cited by 474
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Metadata
- Authors
- Sharafi, A., Kazyak, E., Davis, A. L., Yu, S., Thompson, T., Siegel, D. J., Dasgupta, N. P., & Sakamoto, J.
- Venue
- Chemistry of Materials
- Publisher
- American Chemical Society (ACS)
- Published
- 2017-09-01
- Volume
- 29
- Issue
- 18
- Pages
- 7961-7968
- ISSN
- 0897-4756 (ISSN-L)
- 1520-5002
- OpenAlex
- W2750682527
- Cited by
- 844
- References
- 6
- FWCI
- 28.19
- Type
- journal article
- Language
- en
- Open access
- closed
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- Sharafi, A., Kazyak, E., Davis, A. L., Yu, S., Thompson, T., Siegel, D. J., Dasgupta, N. P., & Sakamoto, J. (2017). Surface Chemistry Mechanism of Ultra-Low Interfacial Resistance in the Solid-State Electrolyte Li7La3Zr2O12. Chemistry of Materials. https://doi.org/10.1021/acs.chemmater.7b03002
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