Crystal Orientation-Dependent Reactivity of Oxide Surfaces in Contact with Lithium Metal
Abstract
Understanding ionic transport across interfaces between dissimilar materials and the intrinsic chemical stability of such interfaces is a fundamental challenge spanning many disciplines and is of particular importance for designing conductive and stable solid electrolytes for solid-state Li-ion batteries. In this work, we establish a surface science-based approach for assessing the intrinsic stability of oxide materials in contact with Li metal. Through a combination of experimental and computational insights, using Nb-doped SrTiO3 (Nb/STO) single crystals as a model system, we were able to understand the impact of crystallographic orientation and surface morphology on the extent of the chemical reactions that take place between surface Nb, Ti, and Sr upon reaction with Li. By expanding our approach to investigate the intrinsic stability of the technologically relevant, polycrystalline Nb-doped lithium lanthanum zirconium oxide (Li6.5La3Zr1.5Nb0.5O12) system, we found that this material reacts with Li metal through the reduction of Nb, similar to that observed for Nb/STO. These results clearly demonstrate the feasibility of our approach to assess the intrinsic (in)stability of oxide materials for solid-state batteries and point to new strategies for understanding the performance of such systems.
- Authors:
-
[1];
[1];
[2];
[1];
- Argonne National Lab. (ANL), Argonne, IL (United States)
- Univ. of Michigan, Ann Arbor, MI (United States)
- Publication Date:
- Research Org.:
- Argonne National Lab. (ANL), Argonne, IL (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V)
- OSTI Identifier:
- 1455046
- Grant/Contract Number:
- AC02-06CH11357
- Resource Type:
- Accepted Manuscript
- Journal Name:
- ACS Applied Materials and Interfaces
- Additional Journal Information:
- Journal Volume: 10; Journal Issue: 20; Journal ID: ISSN 1944-8244
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; Li metal; buried interface; model system; reactivity; solid electrolytes; solid-state batteries; surface science
Citation Formats
Connell, Justin G., Zhu, Yisi, Zapol, Peter, Tepavcevic, Sanja, Sharafi, Asma, Sakamoto, Jeff, Curtiss, Larry A., Fong, Dillon D., Freeland, John W., and Markovic, Nenad M. Crystal Orientation-Dependent Reactivity of Oxide Surfaces in Contact with Lithium Metal. United States: N. p., 2018.
Web. doi:10.1021/acsami.8b03078.
Connell, Justin G., Zhu, Yisi, Zapol, Peter, Tepavcevic, Sanja, Sharafi, Asma, Sakamoto, Jeff, Curtiss, Larry A., Fong, Dillon D., Freeland, John W., & Markovic, Nenad M. Crystal Orientation-Dependent Reactivity of Oxide Surfaces in Contact with Lithium Metal. United States. https://doi.org/10.1021/acsami.8b03078
Connell, Justin G., Zhu, Yisi, Zapol, Peter, Tepavcevic, Sanja, Sharafi, Asma, Sakamoto, Jeff, Curtiss, Larry A., Fong, Dillon D., Freeland, John W., and Markovic, Nenad M. Mon .
"Crystal Orientation-Dependent Reactivity of Oxide Surfaces in Contact with Lithium Metal". United States. https://doi.org/10.1021/acsami.8b03078. https://www.osti.gov/servlets/purl/1455046.
@article{osti_1455046,
title = {Crystal Orientation-Dependent Reactivity of Oxide Surfaces in Contact with Lithium Metal},
author = {Connell, Justin G. and Zhu, Yisi and Zapol, Peter and Tepavcevic, Sanja and Sharafi, Asma and Sakamoto, Jeff and Curtiss, Larry A. and Fong, Dillon D. and Freeland, John W. and Markovic, Nenad M.},
abstractNote = {Understanding ionic transport across interfaces between dissimilar materials and the intrinsic chemical stability of such interfaces is a fundamental challenge spanning many disciplines and is of particular importance for designing conductive and stable solid electrolytes for solid-state Li-ion batteries. In this work, we establish a surface science-based approach for assessing the intrinsic stability of oxide materials in contact with Li metal. Through a combination of experimental and computational insights, using Nb-doped SrTiO3 (Nb/STO) single crystals as a model system, we were able to understand the impact of crystallographic orientation and surface morphology on the extent of the chemical reactions that take place between surface Nb, Ti, and Sr upon reaction with Li. By expanding our approach to investigate the intrinsic stability of the technologically relevant, polycrystalline Nb-doped lithium lanthanum zirconium oxide (Li6.5La3Zr1.5Nb0.5O12) system, we found that this material reacts with Li metal through the reduction of Nb, similar to that observed for Nb/STO. These results clearly demonstrate the feasibility of our approach to assess the intrinsic (in)stability of oxide materials for solid-state batteries and point to new strategies for understanding the performance of such systems.},
doi = {10.1021/acsami.8b03078},
journal = {ACS Applied Materials and Interfaces},
number = 20,
volume = 10,
place = {United States},
year = {Mon Apr 30 00:00:00 EDT 2018},
month = {Mon Apr 30 00:00:00 EDT 2018}
}
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Cited by: 7 works
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Figures / Tables:
Figure 1: (a) LEED and (b) AFM images of an etched and annealed STO(001) surface. (c) AFM image of the same STO(001) surface after Li deposition. Scale bars are 1 μm and height scale units are nm. (d-f) XPS core level spectra before (red) and after (blue) Li deposition showmore »
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Works referencing / citing this record:
Dopant‐Dependent Stability of Garnet Solid Electrolyte Interfaces with Lithium Metal
journal, January 2019
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Figures / Tables found in this record:
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